Cancer is one of the deadliest diseases, and current treatment regimens suffer from limited efficacy, nonspecific toxicity, and chemoresistance. With the advantages of good biocompatibility, large specific surface area, excellent cation exchange capacity, and easy availability, clay minerals have been receiving ever‐increasing interests in cancer treatment. They can act as carriers to reduce the toxic side effects of chemotherapeutic drugs, and some of their own properties can kill cancer cells, etc. Compared with other morphologies clays, layered clay minerals (LCM) have attracted more and more attention due to adjustable interlayer spacing, easier ion exchange, and stronger adsorption capacity. In this review, the structure, classification, physicochemical properties, and functionalization methods of LCM are summarized. The state‐of‐the‐art progress of LCM in antitumor therapy is systematically described, with emphasis on the application of montmorillonite, kaolinite, and vermiculite. Furthermore, the property–function relationships of LCM are comprehensively illustrated to reveal the design principles of clay‐based antitumor systems. Finally, foreseeable challenges and outlook in this field are discussed.
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