Scalable Wire‐Type Asymmetric Pseudocapacitor Achieving High Volumetric Energy/Power Densities and Ultralong Cycling Stability of 100 000 Times

Wire‐shaped asymmetric pseudocapacitors with both pseudocapacitive cathode and anode are promising in facilitating device assembly and provide highly efficient power sources for wearable electronics. However, it is a great challenge to simultaneously obtain high energy and power as well as ultralong cycling life for practical demands of such devices. Herein, a device design with new cathode/anode coupling is proposed to achieve excellent comprehensive performance in a wire‐type quasi‐solid‐state asymmetric pseudocapacitor (WQAP). The hierarchical α‐MnO(2) nanorod@δ‐MnO(2) nanosheet array cathode and MoO(2)@C nanofilm anode are directly grown on flexible tiny Ti wires by well‐established hydrothermal and electrodeposition techniques, which ensures rapid charge/mass transport kinetics and the sufficient utilization of pseudocapacitance. The nanoarray/film electrode also facilitates integration with gel electrolyte of polyvinyl alcohol–LiCl, guaranteeing the durability. The resulting WQAP with 2.0 V voltage delivers high volumetric energy and power densities (9.53 mWh cm(−3) and 22720 mW cm(−3), respectively) as well as outstanding cycling stability over 100 000 times, surpassing all the previously reported WQAPs. In addition, the device can be facilely connected in parallel or in series with minimal internal resistance, and be fabricated at the 1 m scale with excellent flexibility. This work opens the way to develop high‐performance integrated wire supercapacitors.