We report the use of multifunctional dendrimer-entrapped gold nanoparticles (Au DENPs) loaded with gadolinium (Gd) chelator/Gd(III) complexes and surface-modified with thiolated cyclo(Arg-Gly-Asp-Phe-Lys(mpa)) (RGD) peptide for targeted dual-mode computed tomography (CT)/magnetic resonance (MR) imaging of small tumors. In this study, amine-terminated generation 5 poly(amidoamine) dendrimers were used as a nanoplatform to be covalently modified with Gd chelator, RGD via a polyethylene glycol (PEG) spacer, and PEG monomethyl ether. Then the multifunctional dendrimers were used as templates to entrap gold nanoparticles, followed by chelating Gd(III) ions and acetylation of the remaining dendrimer terminal amines. The thus-formed multifunctional Au DENPs (in short, Gd-Au DENPs-RGD) were characterized via different techniques. We show that the multifunctional Au DENPs with a Au core size of 3.8 nm are water-dispersible, stable under different pH (5-8) and temperature conditions (4-50 °C), and noncytotoxic at a Au concentration up to 100 μM. With the displayed X-ray attenuation property and the r1 relaxivity (2.643 mM(-1) s(-1)), the developed Gd-Au DENPs-RGD are able to be used as a dual-mode nanoprobe for targeted CT/MR imaging of an αvβ3 integrin-overexpressing xenografted small tumor model in vivo via RGD-mediated active targeting pathway. The developed multifunctional Gd-Au DENPs-RGD may be used as a promising dual-mode nanoprobe for targeted CT/MR imaging of different types of αvβ3 integrin-overexpressing cancer.