Abstract Peptide-coordination self-assembly demonstrates great potential in the precise design of next-generation theranostic nanodrugs. It has the advantages of high biosafety, versatile system design, easy control over the self-assembled structures, facile incorporation of various functionalities, and greatly enhanced stability of the complex materials as well as their stimuli-responsive assembly and disassembly. All of these merits promote the construction of targeted theranostic systems with highly integrated diagnostic and therapeutic functionalities. This review seeks to provide an up-to-date conclusive observation about the field of peptide-coordination self-assembly for theranostic applications to guide related research. It covers the general principles of peptide-coordination self-assembly for producing structures with controlled morphologies and properties, the strategies for constructing peptide/metal hybrid materials for diagnostic and therapeutic aims, and, more specifically, the strategies and design rules for integrating various functionalities into a single platform for theranostics.