The objective of this account is to summarize our recent progress with functional biosupramolecular systems concisely. The functions covered are artificial photosynthesis, anion transport, and sensing in lipid bilayer membranes. With artificial photosynthesis, the current emphasis is on the construction of ordered and oriented architectures on solid surfaces. Recent examples include the zipper assembly of photosystems with supramolecular n/p-heterojunctions and oriented antiparallel redox gradients. Current transport systems in lipid bilayers reveal new interactions at work. Examples include anion−macrodipole or anion−π interactions. Current attention with membrane-based sensing systems shifts from biosensor approaches with enzymatic signal generation to aptamers (i.e., the DNA version of immunosensing) and differential sensing with dynamic polyion−counterion transporters. The functional diversity accessible with biosupramolecular systems is highlighted, as is the critical importance of cross-fertilization at intertopical convergence zones.