In addition to drugs, natural compounds such as functional food factors have demonstrated great potential for cancer therapy due to their low cost, mild side effects, and common raw materials. However, their short half‐life period, easy decomposition, and lack of targeting severely limit their further development. Metal‐organic frameworks (MOFs) are a new type of porous crystalline materials that are created by combining metal clusters and organic linkers. MOFs have enormous applications, particularly in the biomedical field, due to their ability for pre‐functional design and post‐functional modification. In this mini‐review, we summarize recent research progress on combining MOFs with natural compounds for anti‐cancer performance, which will provide new insights for future research in the biomedical field.