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A novel and green multifunctional nanoplatform as a nanocarrier for drug delivery, cell imaging, and phototherapy has been engineered. The nanoplatform is composed of stabilized carbon spheres (CSs) as cores, a coated polydopamine (PDA) shell, targeted folic acid (FA), and the loaded anticancer drug indocyanine green (ICG), obtaining CSs@PDA-FA@ICG nanocomposites (NCs). The biocompatible PDA shell provided a high fluorescence quenching efficiency and a surface rich in functional groups for anchoring FA for targeting cancer cells. Aromatic ICG could be effectively loaded into the CSs@PDA-FA system via hydrophobic interactions and π-π stacking with a loading efficiency of 58.9%. Notably, the activated NIR fluorescence in an intracellular environment made CSs@PDA-FA@ICG a sensitive "OFF" to "ON" nanoprobe that can be used for NIR imaging. Moreover, compared to ICG alone, the CSs@PDA-FA@ICG NCs could induce efficient photoconversion for simultaneous synergetic photodynamic therapy (PDT) and photothermal therapy (PTT) under a single NIR laser irradiation. The results demonstrated that CSs@PDA-FA@ICG NCs as a targeted and activated nanoplatform provide new opportunities to facilitate the accurate diagnosis of cancer and enhanced treatment efficacy. This work stimulates more interest in the design of the facile surface functionalization strategy to construct other multifunctional nanocomposites, such as nanotubes and nanorods.