For the first time, two types of highly anisotropic, highly transparent wood composites are demonstrated by taking advantage of the macro-structures in original wood. These wood composites are highly transparent with a total transmittance up to 90% but exhibit dramatically different optical and mechanical properties.

Transparent films or substrates are ubiquitously used in photonics and optoelectronics, with glass and plastics as traditional choice of materials. Transparent films made of cellulose nanofibers are reported recently. However, all these films are isotropic in nature. This work, for the first time, reports a remarkably facile and effective approach to fabricating anisotropic transparent films directly from wood. The resulting films exhibit an array of exceptional optical and mechanical properties. The well-aligned cellulose nanofibers in natural wood are maintained during delignification, leading to an anisotropic film with high transparency (≈90% transmittance) and huge intensity ratio of transmitted light up to 350%. The anisotropic film with well-aligned cellulose nanofibers has a mechanical tensile strength of up to 350 MPa, nearly three times of that of a film with randomly distributed cellulose nanofibers. Atomistic mechanics modeling further reveals the dependence of the film mechanical properties on the alignment of cellulose nanofibers through the film thickness direction. This study also demonstrates guided liquid transport in a mesoporous, anisotropic wood film and its possible application in enabling new nanoelectronic devices. These unique and highly desirable properties of the anisotropic transparent film can potentially open up a range of green electronics and nanofluidics.

Highly conductive and mechanically strong microfibers are attractive in energy storage, thermal management, and wearable electronics. Here, a highly conductive and strong carbon nanotube/nanofibrillated cellulose (CNT–NFC) composite microfiber is developed via a fast and scalable 3D‐printing method. CNTs are successfully dispersed in an aqueous solution using 2,2,6,6‐tetramethylpiperidinyl‐1‐oxyl (TEMPO) oxidated NFCs, resulting in a mixture solution with an obvious shear‐thinning property. Both NFC and CNT fibers inside the all‐fiber‐based microfibers are well aligned, which helps to improve the interaction and percolation between these two building blocks, leading to a combination of high mechanical strength (247 ± 5 MPa) and electrical conductivity (216.7 ± 10 S cm−1). Molecular modeling is applied to offer further insights into the role of CNT–NFC fiber alignment for the excellent mechanical strength. The combination of high electrical conductivity, mechanical strength, and the fast yet scalable 3D‐printing technology positions the CNT–NFC composite microfiber as a promising candidate for wearable electronic devices.

We integrated plastic into mesoporous paper to achieve a new type of substrate plastic–paper for high performance optoelectronics.