Triboelectric nanogenerators (TENGs) are an emerging energy-harvesting technology capable of converting mechanical energy into electrical energy. However, triboelectric layers, crucial components of TENGs, are susceptible to mechanical and structural damage in harsh environments, thereby compromising the device's output performance and limiting its applicability. Therefore, developing triboelectric layers with excellent mechanical strength and environmental stability poses a challenge. Inspired by the intricate multiple cross-linking networks present in myofibrillar proteins, a strategy of multiple cross-linking is proposed to prepare conductive special rubbers with outstanding mechanical strength (13.5 MPa), environmental stability, and electrical conductivity (0.86 S m−1) using a “grafting–hydrogenation–cross-linking–filling” process. The multiple cross-linking networks considerably enhanced the rubber's strength by 100 times (0.3–30.3 MPa). Subsequently, these special rubbers are employed as triboelectric layers in accordion-structured TENGs, which demonstrated exceptional electrical output performance with an open-circuit voltage of 723 V and a power density of up to 3.25 W m−2. TENGs can operate stably in a wide range of harsh environments. This study provides a viable strategy for designing TENGs capable of functioning in harsh environments, thereby contributing to sustainable energy solutions.