One of the most fundamental challenges in developing more elaborate self-assembled peptide nanostructures (SPNs) lies in the design of building blocks that are both more complex and relatively easy to synthesize. In this talk, I present the reseaches on self-assembling Janus peptide dendrimers (JPDs), which building blocks have 3-dimensional (3D) structures similar to those of globular proteins. For the reliable and convenient synthesis of JPDs, we devised a novel solid-phase bifurcation synthesis protocol. Because JPD assemblies habor dual multivalency, i.e., supramolecular and unimolecular multivalency, the JPD assembly system enables the statistical selection of nanostructures with high avidity for any desired cell types and possibly any target receptors.