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Abstract The cost‐effective and scalable synthesis and patterning of soft nanomaterial composites with improved electrical conductivity and mechanical stretchability remains challenging in wearable devices. This work reports a scalable, low‐cost fabrication approach to directly create and pattern crumpled porous graphene/NiS₂nanocomposites with high mechanical stretchability and electrical conductivity through laser irradiation combined with electrodeposition and a pre‐strain strategy. With modulated mechanical stretchability and electrical conductivity, the crumpled graphene/NiS₂nanocomposite can be readily patterned into target geometries for application in a standalone stretchable sensing platform. By leveraging the electrical energy harvested from the kinetic motion from wearable triboelectric nanogenerator (TENG) and stored in micro‐supercapacitor arrays (MSCAs) to drive biophysical sensors, the system is demonstrated to monitor human motions, body temperature, and toxic gas in the exposed environment. The material selections, design strategies, and fabrication approaches from this study provide functional nanomaterial composites with tunable properties for future high‐performance bio‐integrated electronics.