Angiogenesis is a vital process for the growth and metastasis of malignant tumor. Visualization of tumor angiogenesis is thus of great importance in the evaluation of biologic aggressiveness as well as monitoring of the response to anti-angiogenic therapy. Herein, we developed a probe based on gold nanoparticles (GNPs) directly surface-functionalized with a tumor-homing cyclized asparagine-glycine-arginine peptide (SH-cNGR) and carboxylpoly(ethylene glycol)thiol (SH-PEG-COOH) Au-S bonds. The obtained GNPs-PEG@cNGR probe was used to target the aminopeptidase-N (APN/CD13), which overexpressed in the endothelium of tumor angiogenesis. The CD13 binding affinities of the peptides were assessed by a receptor binding assay based on HUVEC and HepG2 cell ( fluorescence imaging and X-ray computed tomography (CT)). The tumor targeting efficacy and the distribution of the GNPs-PEG@cNGR were further evaluated in a subcutaneous 4T1 xenograft model by CT imaging and immunohistochemistry study. These results showed that the GNPs-PEG@cNGR rapidly and specifically bound to the tumor vasculature after intravenous injection. Quantitative studies demonstrated that GNPs-PEG@cNGR showed significantly higher and faster tumor uptake after intravenous injection compared to unlabeled GNPs-PEG. Moreover, the distribution of tumor enhancement was consistent with the spatial distribution of angiogenic blood. These results suggest that the designed GNPs-PEG@cNGR probe may serve, in principle, as a promising CT contrast agent for targeted angiogenesis imaging and quantitative analysis.