Biomaterials interfaces are at the heart of new approaches to control cell-surface interactions, and modern surface analytical techniques can now provide molecular-scale information about surface modifications, coverages and patterning or relevant ligands and proteins. These approaches can inform our understanding of the relationship between surface chemistry, surface structure and biological function. Using the biomedical problem of repair to damaged central nervous system tissue as the motivation for biomaterials interface characterization and cell-surface interactions, we will present several approaches to surface modification and surface characterization in conjunction with cell-surface biophysical measurements. The tools for these studies are AFM, XPS, TOF-SIMS and fluorescence microscopy and labeling.