Dendrimers can be obtained in precise molecular weights even at high generations. This feature, as well as the inherent globular shape of high generation dendrimers, makes them ideal candidates for macromolecular biomimetics. In this account, we discuss the synthesis and use of dendrimers that are reminiscent of macromolecular architectures present in nature. In particular, we focus the use of dendrimers in the areas of encapsulation, functionalization, and sequencing.