Dendrimers, a special class of synthetic polymers known for their well-defined ramified structures and unique multivalent cooperativity, hold great promise for various biomedical applications. However, preparation of defect-free dendrimers of high-generation on a large scale remains challenging because of the tedious and time-consuming synthesis as well as difficult purification. To overcome these limitations, an alternative strategy based on self-assembling approach has been developed to construct supramolecular dendrimers using small amphiphilic dendrimer-building units. By virtue of the amphiphilic nature, these small dendrimer-building units self-assemble and form large non-covalent supramolecular dendritic structures that mimic high-generation covalent dendrimers. Here, we present a brief overview of the supramolecular dendrimers developed in our group for the delivery of nucleic acid therapeutics, anticancer drug and imaging agents.