Applications of silicone gel in flexible devices and soft machines require it to maintain excellent stretchability and antifatigue. However, the reported fatigue threshold of traditional silicone gels is in the range of 1–100 J m−2 and the stretchability below 2000 %. Herein, we report a simple strategy for constructing soft polydimethylsiloxane gels, which possesses high stretchability up to 8300 %, and high fatigue resistance (321 J m−2). This is achieved by controlling the ratio of chemical crosslinking and physical entanglement in the polydimethylsiloxane gels. The symbiotic relationship of this combination includes: extending the polymer chains helps them unfold to increase softness and intrinsic toughness; controlling the physical entanglement and chemical cross-linking helps to further increase the tensile rate and fatigue threshold, and adding small-molecule dimethyl PDMS as a solvent further increases fatigue resistance and tensile properties. This work provides a facile approach for developing super-stretchable and anti-fatigue silicone gel, which promises wide range of applicant in flexible devices and soft machines.
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