Ideally, any material used should be nontoxic and produced with safe, inexpensive, and energy‐effective processes. In the case of optically active nanoparticles, this is often not the case, as they are frequently composed of hazardous heavy metals and/or produced with methods far from being environmentally friendly. Herein, the preparation of Ag2S‐based nanoparticles via a simple green synthesis route is explored. Aqueous extracts of roasted coffee are used as sources of coordinating molecules. Optimization of the reaction conditions yields dimeric Ag−Ag2S nanoparticles, whose near‐infrared photoluminescence can be switched on via H2O2‐mediated oxidation. This oxidation transforms suitable photoacoustic contrast agents into fluorescence imaging probes. Theoretical calculations further clarify the role of metallic silver in determining the optical properties of Ag2S. Overall, it is demonstrated that nanomaterials with tangible applicative potential can be prepared via cost‐ and energy‐effective synthesis strategies that entail benign, renewable chemicals.

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