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A novel near-infrared light photothemal-activated H2S-donating nanocomposite hydrogel was developed, through combination of a thermo-labile H2S donor and photothermal nanoparticles in agarose hydrogel. The polyethylenimine dithiocarbamate polymer, a thermo-labile compound, was synthesized as a novel H2S donor. The combination of a thermo-labile hydrogen sulfide donor and photothermal nanoparticles enabled the generation of H2S in agarose hydrogel upon irradiation with near-infrared light. The ability to modulate the photoirradiation for controlled generation and spatiotemporally release of H2S are its specific advantages. This photothermal spatiotemporally controlled H2S-releasing strategy was successfully applied to anti-inflammation treatment in a rat model, demonstrating its utility as a novel H2S-based therapeutic approach.