Linear-dendron (LD) hybrids are macromolecules comprising a linear polymer or oligomer conjugated at one or both termini with branched macromolecules called dendrons. Since their introduction approximately 2 decades ago, tremendous progress has been made in their synthesis, the study of their self-assembly, and toward their application in a variety of fields. This highlight is focused on aqueous assemblies of LD hybrids where function is imparted by the dendron, linear component, or both. These functions include the encapsulation and release of drug molecules, enhancement of cell uptake and targeting of specific tissues, and the stabilization of enzymes for catalysis. In addition, many stimuli-responsive LD hybrids that undergo changes in response to light, enzymes, pH, temperature, redox potential, or even multiple stimuli have been developed. LD hybrids can also be used to form networks via cross-linking reactions. Described here are the structure-property relationships underlying the functions of these materials, along with their potential applications.