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Supramolecular interactions with dynamic, reversible, and directional features enable the design of biomaterials with ordered architectures, tailored morphologies, multiple types of cargo, and controllable functions. Such supramolecular biomaterials are good candidates for oncology applications, as they optimize therapeutic efficacy while minimizing systemic adverse effects. This review summarizes recent advances in intelligent supramolecular biomaterials, with a specific focus on their spatiotemporal control in cancer theranostics. These biomaterials exploit endogenous and exogenous stimuli to trigger their morphological transformation. In particular, their construction approach and working mechanism, which are crucial in guiding tumor theranostics, are elaborated. 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