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One-dimensional nanomaterials have become one of the most available nanoreinforcing agents for developing next-generation high-performance functional self-healing composites owing to their unique structural characteristics and surface electron structure. However, nanoscale control, structural regulation, and crystal growth are still enormous challenges in the synthesis of specific one-dimensional nanomaterials. Here, oxygen-defective MoO3–xnanowires with abundant surface dynamic bonding were successfully synthesized as novel nanofillers and photothermal response agents combined with a polyurethane matrix to construct composite elastomers, thus achieving mechanically enhanced and self-healing properties. Benefiting from the surface plasmon resonance of the MoO3–xnanowires and interfacial multiple dynamic bonding interactions, the composite elastomers demonstrated strong mechanical performance (with a strength of 31.45 MPa and elongation of 1167.73%) and ultrafast photothermal toughness self-healing performance (20 s and an efficiency of 94.34%). The introduction of MoO3–xnanowires allows the construction of unique three-dimensional cross-linked nanonetworks that can move and regulate interfacial dynamic interactions under 808 nm infrared laser stimulation, resulting in controlled mechanical and healing performance. Therefore, such special elastomers with strong photothermal responses and mechanical properties are expected to be useful in next-generation biological antibacterial materials, wearable devices, and artificial muscles.