LAUSR

While photoluminescent graphene quantum dots (GQDs) have long been considered very suitable for bioimaging owing to their protein‐like size, superhigh photostability and in vivo long‐term biosafety, their unique and crucial bioimaging applications in vivo remain unreachable. Herein, planted GQDs are presented as an excellent tool for in vivo fluorescent, sustainable and multimodality tumor bioimaging in various scenarios. The GQDs are in situ planted in the poly(ethylene glycol) (PEG) layer of PEGylated nanoparticles via a bottom‐up molecular approach to obtain the NPs‐GQDs‐PEG nanocomposite. The planted GQDs show more than four times prolonged blood circulation and 7–8 times increased tumor accumulation than typical GQDs in vivo. After accessible specificity modification, the multifunctional NPs‐GQDs‐PEG provides targeted, multimodal molecular imaging for various tumor models in vitro or in vivo. Moreover, the highly photostable GQDs enable long‐term, real‐time visualization of the local pharmacokinetics of NPs in vivo. Planting GQDs in PEGylated nanomedicine offers a new strategy for broad in vivo biomedical applications of GQDs.