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With the combination of high flexibility and thermal property, thermally conductive elastomers have played an important role in daily life. However, traditional thermally conductive elastomers display limited stretchability and toughness, seriously restricting their further development in practical applications. Herein, a high-performance composite is fabricated by dispersing room-temperature liquid metal microdroplets (LM) into a polyborosiloxane elastomer (PBSE). Due to the unique solid–liquid coupling mechanism, the LM can deform with the PBSE matrix, achieving higher fracture strain (401%) and fracture toughness (2164 J/m2). Meanwhile, the existence of LM microdroplets improves the thermal conductivity of the composite. Interestingly, the LM/PBSE also exhibits remarkable anti-impact, adhesion capacities under complex loading environments. As a novel stretchable elastomer with enhanced mechanical and thermal behavior, the LM/PBSE shows good application prospects in the fields of thermal camouflages, stretchable heat-dissipation matrixes, and multifunctional shells for electronic devices.

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This work illustrates a “soft‐toughness” coupling design method to integrate the shear stiffening gel (SSG), natural leather, and nonwoven fabrics (NWF) for preparing leather/MXene/SSG/NWF (LMSN) composite with high anti‐impact protecting, piezoresistive sensing, electromagnetic interference (EMI) shielding, and human thermal management performance. Owing to the porous fiber structure of the leather, the MXene nanosheets can penetrate leather to construct a stable 3D conductive network; thus both the LM and LMSN composites exhibit superior conductivity, high Joule heating temperature, and an efficient EMI shielding effectiveness. Due to the excellent energy absorption of the SSG, the LMSN composites possess a huge force‐buffering (about 65.5%), superior energy dissipation (above 50%), and a high limit penetration velocity of 91 m s−1, showing extraordinary anti‐impact performance. Interestingly, LMSN composites possess an unconventional opposite sensing behavior to piezoresistive sensing (resistance reduction) and impact stimulation (resistance growing), thus they can distinguish the low and high energy stimulus. Ultimately, a soft protective vest with thermal management and impact monitoring performance is further fabricated, and it shows a typical wireless impact‐sensing performance. This method is expected to have broad application potential in the next‐generation wearable electronic devices for human safeguarding.