Metal-phenolic networks (MPNs) have shown promising potential in biomedical applications since they provide a rapid, simple and robust way to construct multifunctional nanoplatforms. As a novel nanomaterial self-assembled from metal ions and polyphenols, MPNs can be prepared to assist the theranostics of cancer owing to their bio-adhesiveness, good biocompatibility, versatile drug loading, and stimuli-responsive profile. This Critical Review aims to summarize recent progress in MPN-based nanoplatforms for multimodal tumor therapy and imaging. First, the advantages of MPNs as drug carriers are summarized. Then, various tumor therapeutic modalities based on MPNs are introduced. Next, MPN-based theranostic systems are reviewed. In terms of in vivo applications, specific attention is paid to their biosafety, biodistribution, as well as excretion. Finally, some problems and limitations of MPNs are discussed, along with a future perspective on the field.