ABSTRACT Atomic‐level structural engineering represents a powerful paradigm for tailoring layered nanomaterials (LNs) toward advanced cancer theranostics, enabling precise control of physicochemical properties to overcome the limitations of conventional nanoplatforms. This review provides a comprehensive overview of the latest advances in engineering LNs, including layered metal oxides, layered double hydroxides, transition metal dichalcogenides, graphene, layered silicates, graphitic carbon nitride, metal carbides and nitrides, and other layered frameworks for cancer diagnosis and therapy. Five representative atomic‐level engineering strategies are discussed, including crystal phase engineering, defect engineering, heteroatom doping, interlayer spacing engineering, and crystalline‐to‐amorphous phase engineering. For each strategy, the underlying mechanisms, representative synthetic approaches, and their roles in optimizing theranostic performance, such as photothermal conversion, reactive oxygen species generation, and multimodal imaging, are critically discussed. Crucially, the advantages and inherent limitations of these engineering strategies are comparatively evaluated to provide a balanced perspective on their practical applicability. Finally, key challenges toward clinical translation, including structural stability, biosafety, and scalability, are highlighted. Future directions are proposed for developing intelligent, adaptive, and personalized LN‐based nanomedicines for precision oncology.
Pan et al. (2026) studied this question.