Pseudocapacitive storage of Zn2+ in nanostructured molybdenum disulfide (MoS2) is expected to break through the limitations of sulfide in monovalent or multivalent ions storage; however, the deficiency of theoretical guidance and experimental strategies that enable rational design of MoS2 as a kind of cathode material towards aqueous zinc-ion batteries. Herein, we firstly establish guiding theory in order to design pseudocapacitive MoS2-based cathode in the light of the first-principles calculation, and then propose a simple and effective one-pot template-free solvothermal method to synthesize 1T phase-dominated MoS2 cathode with low crystallinity. Through this method, MoS2 cathode delivers an exceptional reversible capacity of 233 mAhg−1 at 0.05 A g−1, especially at 0.1 A g−1, the stability can achieve >150 cycles, and maintains 84 % capacity retention after 2100 cycles at 5 A g−1. Experimental and theoretical analysis show that such extraordinary pseudocapacitive contribution determines by the synergistic effects in the activated and stable metallic phase, abundant lattice defects and larger interlayer spacing in the rag-like MoS2 cathode. The revealed origin of highly pseudocapacitive Zn2+ storage and design principle for MoS2-based cathode facilitate the design of a variety of efficient cathodes.