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Intracellular self‐assembly (ISA) is a versatile and powerful strategy for in situ constructing sophisticated and functional supramolecular nanostructures, which has been widely applied in biomedicine and biomedical engineering. Among the common building blocks for ISA, peptides have attracted increasingly attention due to their intrinsic bioactivity, biocompatibility, and biodegradability. Particularly, by conjugating functional motifs (e.g., probes or drugs) to peptides to yield the peptide conjugates, the latter show enhanced stability and efficiency, and probably new functions. In recent years, employing ISA of peptide conjugates for tumor imaging and treatment has achieved great progresses. Therefore, the recent progress of ISA of peptide conjugates is summarized in this progress report. Moreover, several examples of ISA of peptide conjugates for other important imaging or therapeutic applications are also …