Two complementary strategies can be employed in the fabrication of molecular biomaterials. In the ‘top-down’ approach, biomaterials are generated by stripping down a complex entity into its component parts. This contrasts with the ‘bottom-up’ approach, in which materials are assembled molecule by molecule and in some cases even atom by atom to produce novel supramolecular architectures. The latter approach is likely to become an integral part of nanomaterials manufacture and requires a deep understanding of individual molecular building blocks, their structures, assembling properties and dynamic behaviors. Two key elements in molecular fabrication are chemical complementarity and structural compatibility, both of which confer the weak and noncovalent interactions that bind building blocks together during self-assembly. Significant advances have been achieved at the interface of biology and materials science, including the fabrication of nanofiber materials for 3-D cell cultures, tissue engineering and regenerative medicine, the peptide detergents for stabilizing, and crystallizing membrane proteins as well as nanocoating molecular for cell organizations. Molecular fabrications of nanobiomateirals have fostered diverse scientific discoveries and technological innovations. Shuguang Zhang made a serendipitous discovery of self-assembling peptides from studying yeast protein, zuotin. He subsequently conceptualized, developed and commercialized diverse self-assembling peptide materials including peptide nanofibers, functional peptide ink, peptide molecular switches and antennae, peptide surfactants/detergents. These self-assembling peptides materials have a broad spectrum of uses, ranging from nanofiber scaffold hydrogel for 3-D tissue cell culture, tissue repair, tissue engineering and regenerative medicine; biochips for direct printing, anchoring and patterning molecules and cells; and peptides for solubilizing, stabilizing and crystallizing membrane proteins. Using systematic and molecular engineering approach, he and his students, postdocs and colleagues opened a new avenue to fabricate novel nanobiological materials from bottom up through molecular self-assembly.