Molecular and supramolecular understanding of the architecture of biological systems, and in particular membranes, can provide an extraordinary source of inspiration for making ‘intelligent’ nanostructures, based on the self-assembly properties of biological molecules. Bioelectronic interfacing between living and inert matter constitutes one of the most promising areas of development in nanobiotechnology. The present chapter is particularly concerned with the description of biological membranes and the self-association properties of the molecules making them up. These provide the basis for a natural and spontaneous formation of structure, which can be used to develop biomimetic membranes and a wide range of nanostructured protein–lipid structures with undeniable scope for application in the field of nanobiotechnology, e.g., lipid nanoparticles, encapsulation and delivery of medicines, targeting, molecular sorting, surface functionalisation, nanobiosensors, etc.