Conventional cathode material synthesis processes (sol–gel, hydrothermal, solid state reactions, and so on) are widely used in aqueous zinc ion battery research, which often requires lengthy, multistage steps involving high temperatures. Herein, a novel plasma‐assisted hydrothermal (PAHT) synthesis has been developed to synthesize 2D & 3D water‐intercalated vanadium oxide (WiVO) nanosheet clusters at low temperature (<200 °C) in a rapid manner (<80 min) with great cathode nanostructure controllability. The resultant WiVO nanosheet clusters exhibit an expanded lattice spacing of 1.23 nm, induced by water intercalation, which enhances Zn ion diffusion kinetics. As a result, 3D WiVO nanosheet clusters achieve a high capacity of 324 mAh g − 1 at 0.1 A g − 1 , and maintaining 95.8% cycle retention after 4000 cycles at 10A g −1 , demonstrating superior aqueous zinc ion batteries (AZIB) performances to anhydrous V 2 O 5 & 2D WiVO nanosheets, backed up by rigorous density functional theory calculations and molecular dynamics simulations, elucidating the enhanced AZIB performances of WiVO 3D nanosheet clusters. Universality of the PAHT method is validated through the synthesis of 3D WiVO nanosheet clusters with comparable cell performance using various vanadium‐based precursors. Furthermore, the electrochemical degradation process of 2D & 3D nanosheet‐based cathode is also explored and the importance of nanosheet clustering, which impedes the degradation process, is demonstrated.