To achieve the optimal performances of flexible pressure devices, the current approaches typically involve extensive experimental trials. However, such methods lack guidance from theoretical models in a positive fashion, not only introducing unpredictability and uncertainty into results but also potentially limiting the applicability of any achieved advancements to the alternative material systems. Here, an electrical-mechanical design model, combining density functional theory and molecular dynamics simulations, was proposed for calculating the specific capacitance and mechanical strength of various modified MXene films. Based on which, the optimal hybrid film entailed the cross-linking of holey reduced graphene oxide and MXene via cysteamine was prepared. This film, upon electromechanical characterizations, has effectively overcome the issues of MXene self-stacking and brittleness, thus validating the conclusions of theoretical predictions. Subsequently, the proposed film was integrated as electrode into a pseudocapacitive pressure sensor, achieving highly sensitivity (∼143,258 kPa−1) and mechanical stability (with capacitance drift below 1.2 % after 10,000-repeated test). Ultimately, the fabricated sensors were developed into sound collection system and robotic skins, respectively, to achieve recognition of distinctive sounds and stable perception of gravity. The calculation-based approach holds enormous potential for the design of two-dementional materials-based pressure sensors.
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