A strategy is presented to control the disassembly of nanogels using near‐infrared light. Novel diselenide‐cross‐linked nanogels with a newly synthesized diselenide cross‐linker are prepared. Indocyanine green is incorporated into nanogels to trigger the cleavage of diselenide bond through generating reactive oxygen species. The appropriate control of illumination allows for on‐demand degradation of nanogels and controlled drug release.