Gold nanoparticles (GNPs) are promising nanomaterials for various biomedical applications owing to their remarkable optical properties and biocompatibility. However, their interfacial properties require modification for practical use in such applications. Herein, a simple method for modifying the surface of GNPs with polydopamine (PDA) to serve as a scaffold for the subsequent polymerization of hyperbranched polyglycerol (HPG) is reported. GNPs were first coated with PDA (GNP-PDA), and then ring-opening chemistry was used at this interface to modify GNP-PDA with HPG (GNP-PDA-HPG). The produced GNP-PDA-HPG shows not only excellent dispersibility in a salt-containing solution but also strong resistance to aggregation in high- and low-pH solutions, even after 10 days. Moreover, we demonstrate a one-pot method for functionalizing GNP-PDA with HPG and either COOH or trimethylammonium. Finally, we conjugated the trimethylammonium-functionalized GNP-PDA-HPG with fluorescent nanodiamonds to investigate the photothermal ability of the functional GNPs.