Flexible and wearable electronics are attracting wide attention due to their potential applications in wearable human health monitoring and care systems. Carbon materials have combined superiorities such as good electrical conductivity, intrinsic and structural flexibility, light weight, high chemical and thermal stability, ease of chemical functionalization, as well as potential mass production, enabling them to be promising candidate materials for flexible and wearable electronics. Consequently, great efforts are devoted to the controlled fabrication of carbon materials with rationally designed structures for applications in next‐generation electronics. Herein, the latest advances in the rational design and controlled fabrication of carbon materials toward applications in flexible and wearable electronics are reviewed. Various carbon materials (carbon nanotubes, graphene, natural‐biomaterial‐derived carbon, etc.) with controlled micro/nanostructures and designed macroscopic morphologies for high‐performance flexible electronics are introduced. The fabrication strategies, working mechanism, performance, and applications of carbon‐based flexible devices are reviewed and discussed, including strain/pressure sensors, temperature/humidity sensors, electrochemical sensors, flexible conductive electrodes/wires, and flexible power devices. Furthermore, the integration of multiple devices toward multifunctional wearable systems is briefly reviewed. Finally, the existing challenges and future opportunities in this field are summarized.

A carbonized plain-weave silk fabric is fabricated into wearable and robust strain sensors, which can be stretched up to 500% and show high sensitivity in a wide strain range. This sensor can be assembled into wearable devices for detection of both large and subtle human activities, showing great potential for monitoring human motions and personal health.

The rational design of high‐performance flexible pressure sensors attracts attention because of the potential applications in wearable electronics and human–machine interfacing. For practical applications, pressure sensors with high sensitivity and low detection limit are desired. Here, ta simple process to fabricate high‐performance pressure sensors based on biomimetic hierarchical structures and highly conductive active membranes is presented. Aligned carbon nanotubes/graphene (ACNT/G) is used as the active material and microstructured polydimethylsiloxane (m‐PDMS) molded from natural leaves is used as the flexible matrix. The highly conductive ACNT/G films with unique coalescent structures, which are directly grown using chemical vapor deposition, can be conformably coated on the m‐PDMS films with hierarchical protuberances. Flexible ACNT/G pressure sensors are then constructed by putting two ACNT/G/PDMS films face to face with the orientation of the ACNTs in the two films perpendicular to each other. Due to the unique hierarchical structures of both the ACNT/G and m‐PDMS films, the obtained pressure sensors demonstrate high sensitivity (19.8 kPa−1, <0.3 kPa), low detection limit (0.6 Pa), fast response time (<16.7 ms), low operating voltage (0.03 V), and excellent stability for more than 35 000 loading–unloading cycles, thus promising potential applications in wearable electronics.

Recent years have witnessed the explosive development of electronic skin. Highly sensitive pressure sensing is one of the primary abilities of electronic skin. To date, most of the reported skin‐like pressure sensors are based on nanomaterials and microstructured polydimethylsiloxane (PDMS) films, limiting their wide practical applications due to the unknown biotoxicity and the redundant fabrication procedure. A cost‐effective, large‐area‐capable, and biocompatible approach for fabrication of high‐performance skin‐like pressure sensors is highly desired. Silk fibroin (SF) is a natural protein that has recently drawn great attention due to its application as the substrate for flexible electronics. Here, the fabrication of skin‐like pressure sensors is demonstrated using SF‐derived active materials. Flexible and conformal pressure sensors can be fabricated using transparent carbonized silk nanofiber membranes (CSilkNM) and unstructured PDMS films through a cost‐effective and large‐scale capable approach. Due to the unique N‐doped carbon nanofiber network structure of CSilkNM, the obtained pressure sensor shows superior performance, including ultrahigh sensitivity (34.47 kPa−1) for a broad pressure range, an ultralow detection limit (0.8 Pa), rapid response time (<16.7 ms), and high durability (>10 000 cycles). Based on its superior performance, its applications in monitoring human physiological signals, sensing subtle touch, and detecting spatial distribution of pressure are demonstrated.

Recent years have witnessed the booming development of flexible strain sensors. To date, it is still a great challenge to fabricate strain sensors with both large workable strain range and high sensitivity. Cotton is an abundant supplied natural material composed of cellulose fibers and has been widely used for textiles and clothing. In this work, the fabrication of highly sensitive wearable strain sensors based on commercial plain weave cotton fabric, which is the most popular fabric for clothes, is demonstrated through a low‐cost and scalable process. The strain sensors based on carbonized cotton fabric exhibit fascinating performance, including large workable strain range (>140%), superior sensitivity (gauge factor of 25 in strain of 0%–80% and that of 64 in strain of 80%–140%), inconspicuous drift, and long‐term stability, simultaneously offering advantages of low cost and simplicity in device fabrication and versatility in applications. Notably, the strain sensor can detect a subtle strain of as low as 0.02%. Based on its superior performance, its applications in monitoring both vigorous and subtle human motions are demonstrated, showing its tremendous potential for applications in wearable electronics and intelligent robots.

Wearable sweat analysis devices for monitoring of multiple health-related biomarkers with high sensitivity are highly desired for noninvasive and real-time monitoring of human health. Here, we report a flexible sweat analysis patch based on a silk fabric–derived carbon textile for simultaneous detection of six health-related biomarkers. The intrinsically N-doped graphitic structure and the hierarchical woven, porous structure provided the carbon textile good electrical conductivity, rich active sites, and good water wettability for efficient electron transmission and abundant access to reactants, enabling it to serve as an excellent working electrode in electrochemical sensors. On the basis of the above, we fabricated a multiplex sweat analysis patch that is capable of simultaneous detection of glucose, lactate, ascorbic acid, uric acid, Na+, and K+. The integration of selective detectors with signal collection and transmission components in this device has enabled us to realize real-time analysis of sweat.

Air filtration in the free molecular flow (FMF) regime is important and challenging because a higher filtration efficiency and lower pressure drop are obtained when the fiber diameter is smaller than the gas mean free path in the FMF regime. In previous studies, FMF conditions have been obtained by increasing the gas mean free path through reducing the pressure and increasing the temperature. In the case of carbon nanotubes (CNTs) with nanoscale diameters, it is possible to filtrate in the FMF regime under normal conditions. This paper reviews recent progress in theoretical and experimental studies of air filtration in the FMF regime. Typical structure models of high-efficiency particulate (HEPA) air filters based on CNTs are introduced. The pressure drop in air filters operated in the FMF regime is less than that predicted by the conventional air filtration theory. The thinnest HEPA filters fabricated from single-walled CNT films have an extremely low pressure drop. CNT air filters with a gradient nanostructure are shown to give a much better filtration performance in dynamic filtration. CNT air filters with a hierarchical structure and an agglomerated CNT fluidized bed air filter are also introduced. Finally, the challenges and opportunities for the application of CNTs in air filtration are discussed.

Conspectus Soft bioelectronics that could be integrated with soft and curvilinear biological tissues/organs have attracted multidisciplinary research interest from material scientists, electronic engineers, and biomedical scientists. Because of their potential human health-related applications, soft bioelectronics require stringent demands for biocompatible components. Silk, as a kind of well-known ancient natural biopolymer, shows unique combined merits such as good biocompatibility, programmable biodegradability, processability into various material formats, and large-scale sustainable production. Such unique merits have made silk popular for intensive design and study in soft bioelectronics over the past decade. Due to the development of fabrication techniques in material processing and progress in research, silk has been engineered into a variety of advanced materials including silk fibers/textiles, nanofibers, films, hydrogels, and aerogels. Natural and regenerated silk materials can also be transformed into intrinsically nitrogen-doped and electrically conductive carbon materials, due to their unique molecular structure and high nitrogen content. The rich morphologies and varied processing options for silk materials can furnish transformed carbon materials with well-designed structures and properties. The favorable and unique material merits of silk materials and silk-derived carbon materials offer potential applications in soft electronics. Based on commercial silk fibers/textiles and the availability of re-engineered silk materials with versatile technological formats, functional soft electronics have been explored with silk as flexible biosupports/biomatrixes or active components. These soft systems include bioresorbable electronics, ultraconformal bioelectronics, transient electronics, epidermal electronics, textile electronics, conformal biosensors, flexible transistors, and resistive switching memory devices. Silk-derived carbon materials with rationally designed morphologies and structures have also been developed as active components for wearable sensors, electronic skins, and flexible energy devices, which provide novel concepts and opportunities for soft electronics. In this Account, we highlight the unique hierarchical and chemical structure of natural silk fibers, the fabrication strategies for processing silk into materials with versatile morphologies and into electrically conductive carbon materials, as well as recent progress in the development of silk-based advanced materials (silk materials and silk-derived carbon materials) for soft bioelectronics. The design and functionality of soft electronics developed with commercial silk fibers/textiles, re-engineered silk materials, and silk-derived carbon materials as biosubstrate/matrix and active components is introduced in detail. We further discuss future challenges and prospects for developing silk-based soft bioelectronics for wearable healthcare systems. By leveraging the unique advantages of silk-based advanced materials, the design and con...