In recent years, the use of nanocarriers to deliver bioactive peptides has become a new strategy to promote angiogenesis. The aim of this study was to develop a QKCMP peptide delivery system based on triangular DNA origami nanostructure (tDONs) carrier to improve the bioactivity and targeting of the peptide. The main objective of this study was to design and prepare QKCMP peptide-TDOns complexes and to evaluate their angiogenesis promoting effects in vitro and in vivo. tDONs were synthesized and purified, and then QKCMP peptide was loaded into tDONs. A variety of characterization techniques were used to evaluate the physicochemical properties of the complexes, including particle size, morphology, and RNA release efficiency. The effects of QKCMP peptid-TDons on proliferation, apoptosis, migration and angiogenesis of human umbilical vein endothelial cells (HUVEC) were evaluated by CCK8, EdU, Annexin V-FITC/PI, PI staining and Transwell assay. At the same time, its promoting effect on angiogenesis was further verified in zebrafish and mouse models. The successful preparation of QKCMP peptide-TDONS showed good biocompatibility and stability. The results of in vitro experiments showed that QKCMP peptide-TDons significantly promoted HUVEC proliferation, inhibited apoptosis, and activated endothelial cell function. Zebrafish experiments showed that QKCMP peptid-TDons effectively enhanced angiogenesis and promoted rapid repair of carotid vascular endothelium in mouse models.