Hyperbranched polymers, a subclass of dendritic polymers, mimic nature's components such as trees and nerves. Hyperbranched polyglycerol (HPG) is a hyperbranched polyether with outstanding physicochemical properties, including high water-solubility and functionality, biocompatibility, and an antifouling feature. HPG has attracted great interest in the modification of different objects, in particular carbon-based nanomaterials. In this review, recent advances in the synthesis and application of HPG to modify carbon-based nanomaterials, including graphene, carbon nanotubes, fullerene, nanodiamonds, carbon dots, and carbon fibers, are reviewed.