This thesis describes progress towards the fabrication of macroscopically large, organized structures made from anisotropic nanomaterials using evaporative self-assembly. Chapter 1 is a literature overview of the characteristics and applications of solid gold nanostructures followed by a discussion of several important aspects of nanofabrication and a discussion of self-assembly in the context of extracellular matrix and cell culture. Chapter 2 describes the crystallization of gold nanotriangles (AuNTs) into hexagonal close-packed superlattices by slow evaporation and includes a morphological comparison of the crystallization habits of gold nanorods (AuNRs) and AuNTs. Chapter 3 discusses the use of a passive foaming system constructed from commercially available TEM grids to assemble gold nanowires into regular checkerboard or honeycomb patterns by the collision of two-dimensional foam bubbles formed by the grid. Chapter 4 presents evaporatively self-assembled networks of collagen and chitosan along with a detailed examination of their structure, and spatial scale-up to macroscopically large 150 mm2 networks using custom grids. Finally, Chapter 5 discusses the application of the gold nanowire, collagen, and chitosan networks as cell culture scaffolds for hTERT RPE-1 cells. Laser scanning confocal microscopy and scanning electron microscopy were used to image and characterize the aligned cells and live cell imaging was utilized to show that cellular motility can be controlled by highly ordered collagen networks.