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Roll‐to‐roll (R2R) printed electronic devices have great advantages for developing large scale flexible and disposable devices when compared to current Si‐based technology. For practical realization of these advantages, however, R2R printed devices need to surmount device functionality limitations, most urgently high‐power dissipation and poor device stability. To resolve both imperative challenges at once, herein, an all R2R printed complementary metal‐oxide‐semiconductor (CMOS) 1‐bit code generator with spin‐coated multilayer encapsulation method is developed. In order to print CMOS devices by an all‐R2R gravure printing method, electrical amphoteric property of the single walled carbon nanotube (SWCNT) is utilized to fabricate both p‐type and n‐type SWCNT based thin film transistors (TFTs). In addition, printable encapsulating polymeric materials (CYTOP and FG‐3650) are developed to effectively prevent H2O permeation. The resulting CMOS 1‐bit code generator is able to continuously operate for 2 h under ambient conditions without any variation in output voltage and frequency.

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Among several electrocatalysts for energy storage purposes including supercapacitors, metal–organic frameworks (MOFs), and their derivatives have spurred wide spread interest owing to their structural merits, multifariousness with tailor‐made functionalities and tunable pore sizes. The electrochemical performance of supercapacitors can be further enhanced using in situ grown MOFs and their derivatives, eliminating the role of insulating binders whose “dead mass” contribution hampers the device capability otherwise. The expulsion of binders not only ensures better adhesion of catalyst material with the current collector but also facilitates the transport of electron and electrolyte ions and remedy cycle performance deterioration with better chemical stability. This review systematically summarizes different kinds of metal–ligand combinations for in situ grown MOFs and derivatives, preparation techniques, modification strategies, properties, and charge transport mechanisms as freestanding electrode materials in determining the performance of supercapacitors. In the end, the review also highlights potential promises, challenges, and state‐of‐the‐art advancement in the rational design of electrodes to overcome the bottlenecks and to improve the capability of MOFs in energy storage applications.

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In our daily lives, electrochemical energy storage technology is of great importance due to our dependence on renewable energy sources (such as solar, wind, geothermal, tidal, and biofuel energy), portable electronics, and forecast of the tremendous markets for electrification of transportation in the near future. [1][2][3][4] The electricity (electric power) can be electrochemically stored in batteries, fuel cells, and electrochemical supercapacitors (SCs). [5,6] Among these electrical energy storage (EES) devices, SCs have attracted more attention due to their higher charge-discharge efficiency, outstanding power density, and significant cyclic stability. [7][8][9][10] In the operation of SCs, there are two types of charge storage mechanisms such as 1) electrical double-layer capacitors (EDLCs) and 2) pseudocapacitors, i.e., Faradaic redox reactions stored the charge. [11] Moreover, in recent years, hybrid capacitors are developed, which consists of an electrode for EDLCs and a battery electrode. [12,13] In last two decades, it was investigated that pseudocapacitors can yield 10-100 times higher specific capacitance than EDLCs. [14,15] For pseudocapacitors, the most commonly utilized electrode materials are transition-metal oxides [16][17][18] and conducting polymers such as polyaniline, polythiophene, and polypyrrole. [19][20][21] The pseudocapacitors based on conducting polymers are more cost-effective than transitionmetal oxides but displayed delayed behavior of Faradaic redox reactions leading to lower power density than EDLCs, swelling of electrodes, which, in turn, hamper the cycle-life stability of the SCs. [22,23] To overcome these drawbacks, in recent decade energy storage devices based on organic molecule electrodes (OMEs) have been developed. [24] Although the OMEs are very good, inexpensive, and green alternative electrode materials, their performance is not up to the mark when compared to inorganic counterparts. [25] Researchers overcome these limitations by fabricating electrode materials using organic molecules with desired properties and conducting carbon scaffolds. The carbon scaffolds are modified with the organic compounds via noncovalent interactions such as π-π stacking or covalent chemical bond formation. [26] Thus, the organic compounds are anchored on carbon materials, which, in turn, prevent their migration in

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