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Multi‐dimensional force sensing that combines intensity, location, area and the like could gather a wealth of information from mechanical stimuli. Developing materials with force‐induced optical and electrical dual responses would provide unique opportunities to multi‐dimensional force sensing, with electrical signals quantifying the force amplitude and the luminescence output providing spatial distribution of force. However, the reliance on external power supply and high‐energy excitation source brings significant challenges to the applicability of multi‐dimensional force sensors. Here we reported the mechanical energy‐driven and sunlight‐activated materials with force‐induced dual responses, and investigated the underlying mechanisms of self‐sustainable force sensing. Theoretical analysis and experimental data unraveled that trap‐controlled luminescence and interfacial electron transfer play a major role in force‐induced optical and electrical output. These materials were manufactured into pressure sensor with renewable dual‐mode output for quantifying and visualization of pressures by electrical and optical output, respectively, without power supply and high‐energy irradiation. The quantification of tactile sensation and stimuli localization of mice highlighted the multi‐dimensional sensing ability of the sensor. Overall, this self‐powered pressure sensor with multimodal output provides more modalities of force sensing, poised to change the way that intelligent devices sense with the world. [ABSTRACT FROM AUTHOR]