Synthesized melanin nanoparticles (SMNPs) are used as advanced photothermal materials. However, their internal structures are complex and disordered, and tuning the photothermal performance of nanoparticles is still a hot spot of concern. This article presents thionin (Th)‐doped SMNPs, namely Th‐SMNPs, which are the first SMNPs formed using the one‐pot polymerization of Th with Levodopa. Th can undergo Michael addition and Schiff base reaction between indole dihydroxy/indolequinone and their oligomers to form donor–acceptor pairs in the structure to modulate the photothermal performance of SMNPs. Structural and spectroscopic analyses and density functional theory simulations further confirm the existence of the donor–acceptor structure. Th‐SMNPs exhibit excellent total photothermal efficiency (34.49%) in the near‐infrared region (808 nm), which is a 60% improvement compared to SMNPs. This allows Th‐SMNPs to exhibit excellent photothermal performance at low power 808 nm laser irradiation. Meanwhile, Th not only enhances the photothermal properties of SMNPs, but also imparts photodynamic effects to SMNPs. Th‐SMNPs can produce 1O2 under 660 nm laser irradiation. A dual‐function photothermal and photodynamic textile named Th‐SMNPs@cotton is constructed based on Th‐SMNPs, which can act as a rapid photothermal/photodynamic sterilization and is promising for wound healing treatment of bacterial infections under low‐power dual laser irradiation.
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