The MnO2-based aqueous Zn cell can meet the requirements of safety, flexibility, and low cost for portable/wearable electronics; however, its low intrinsic conductivity, weak kinetics, and poor high-loading capacity restrict its practical performance. In this study, the synergistic architecture of MoS2-loaded, oxygen-defect-rich MnO2-x nanocrystals with a carbon coating (M-PM2-x-H2 aerogel) was prepared. As corevealed by various characterizations, this synergistic design not only improves the electronic/ionic conductivity but also motivates the conversion kinetics of the surficial electrochemical reaction. As a result, the M-PM2-x-H2 cathode delivers a much improved capacity of 567 mA h·g-1 at 0.1 A·g-1 and shows a high capacity retention of 176% after 150 cycles at 0.5 A·g-1. More impressively, the high areal loading (3.97 mg·cm-1) of the M-PM2-x-H2 electrode also displays a high capacity of 367 mA h·g-1 at 0.1 A·g-1. In addition, the derived all-solid-state cell exhibits excellent flexibility and safety under the conditions of weight loading, cutting, and bending.