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Following the wisdom of nature to assemble functional candidates into exquisite nanoarchitectures is emerging as a promising field of research and has been widely applied in biomedical sciences. Owing to their excellent properties of structural controllability, functional diversity, dynamic adjustability, and prominent biocompatibility, the self-assembled nanoarchitectures come to play a pivotal role in fighting against cancer. This review outlines the most up-to-date developments in constructing phototherapeutic nanomaterials for photodynamic and photothermal therapy (PDT and PTT) of tumors, with emphasis on design ideas, building blocks, and advantageous characteristics of self-assembly. The prominent activities of cancer therapy obtained by these photoinduced nanotheranostics are also explored in-depth, together with the connections between the specific nanostructures and unique features, providing a …