Magnetohydrodynamic Driven Electrodeposited Polypyrrole/NiCo 2 S 4 as Cathode and MoS 2 /Ti 3 C 2 T x MXene as Anode for Flexible Solid‐State Asymmetric Microsupercapacitor

ABSTRACT The customization of material properties during synthesis is crucial for microsupercapacitors performance, influencing morphology, porosity, and charge transport. This work designed an asymmetric microsupercapacitor (AMSC) with a cathode constituting a polypyrrole/NiCo 2 S 4 (PPy/NCS) composite, deposited with magnetic field assistance, and a MoS 2 /Ti 3 C 2 T x MXene hybrid anode synthesized hydrothermally. The magneto‐electrodeposition process triggers magnetohydrodynamic effects, allowing controlled nucleation and growth, resulting in a porous, interconnected nanosheet architecture of PPy/NCS with diffusion‐controlled faradaic behavior. Theoretical calculations supported experimental findings, showing enhanced density of states and increased quantum capacitance for PPy/NCS. Conversely, the MoS 2 /Ti 3 C 2 T x anode offers high electrical conductivity and increased interlayer spacing, thus promoting rapid ion transport and mixed charge storage kinetics. The AMSC device achieved an extended operating voltage window of 1.6 V, an areal specific capacity of 12.8 mC cm −2 at 0.3 mA cm −2 , and excellent energy–power characteristics, with 90% cycling stability over 10,000 charge‐discharge cycles. It showed mechanical flexibility under various deformation angles and potential for powering low‐voltage devices. This superior performance is due to diffusion‐controlled redox reactions at the cathode, balanced by capacitive contributions at the anode. This work highlights synthesis‐driven property modulation and magneto‐electrodeposition as promising methods for developing advanced electrode materials for next‐generation microscale energy storage systems.