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Molybdenum disulfide (MoS2) has significant potential in aqueous zinc-ion batteries (AZIBs) due to its unique layered structure and adjustable layer spacing. However, the electrochemical performance remains unsatisfactory primarily due to the limited interlayer spacing. Here, a composite material consisting of MoS2 nanosheets with expanded interlayer spacing and intercalated surfactant polyethylene glycol (PEG) is proposed as a cathode material for AZIBs. The results indicate that PEG is intercalated into the layered structure of MoS2, resulting in a significant expansion of the MoS2 layer spacing (from 0.62 to 0.95 nm). The PEG effectively mitigates the agglomeration during MoS2 growth, promotes the 2H to 1T phase conversion in MoS2 (about 60% of 1T phase content), provides more active sites for electrochemical reactions, reduces electron transfer resistance, and shortens diffusion distance of zinc ions. During the process of charging and discharging, the intercalated PEG molecules serve as "pillars" to provide structural support for MoS2 layers, thereby enhancing their stability. The pseudocapacitive behavior of the MoS2-PEG is promoted by the combination of these aforementioned advantages. Consequently, the MoS2-PEG composite electrode exhibited a discharge capacity of 123.4 mAh·g−1 at a current density of 1.0 A g−1 and maintained a capacity retention of 83.5% after 200 cycles, while pure MoS2 only displayed a reversible capacity of 71.5 mAh·g−1 under identical conditions. This study provides a reference for the development of MoS2 as a cathode material for AZIBs. [ABSTRACT FROM AUTHOR]