Activating Ion Channels in Collapsed Hydrogel Derived Densified MXene Films with Cellulose Nanofibers to Overcome the Areal Versus Volumetric Capacitance Trade‐Off

Abstract Concomitant achievement of all three performance pillars of a supercapacitor device, namely gravimetric, areal, and volumetric capacitance is a grand challenge. Nevertheless, its fulfilment is indispensable for commercial usage. Although, high compactness is the fundamental requirement to achieve high volumetric performance, it severely affects ion transportation in thick electrodes. Such trade‐off makes it extremely challenging to realize very high areal and volumetric performance simultaneously. Here, a collapsed hydrogel strategy is introduced to develop MXene/cellulose nanofiber (CNF) based densified electrodes that offer excellent ion transportation despite a massive increase in areal mass loading (>70 mg cm −2 ). Quasi‐oriented MXene/CNF (MXCF) hydrogels are produced through an electric field‐guided co‐assembly technique. Ambient dehydration of these hydrogels incorporates numerous pores in the resultant compact electrodes due to crumpling of the MXene sheets, while CNF ensures connectivity among the locally blocked pores in different length scales. The resultant collapsed MXCF densified electrode shows a remarkably high areal capacitance of 16 F cm −2 while simultaneously displaying a high volumetric capacitance of 849.8 F cm −3 at an ultrahigh mass loading of up to 73.4 mg cm −2 . The universality of strategy, including the co‐assembly of hydrogel and its collapse, is further demonstrated to develop high‐performance asymmetric and wearable devices.