Organoalkoxysilanes, (i.e. {[(RO)xSi]y(R)z} where x, y, and z are 1, 2, or 3 and x + z = 4), are important chemical precursors widely used to make organic-functionalized solid-state inorganic materials. Their covalently linked organic group, R-, and polymerizable silyl moieties, [(RO)xSi-] make them well-suited as precursors for organosilica materials or organic-functionalized monolayers synthesized by hydrolysis and condensation on otherwise unfunctionalized metal oxides surfaces. The introduction of organic functional groups into inorganic solid-state structures can greatly extend the chemical and physical properties of inorganic materials. That is, properties such as hydrophobicity and the reactivity of inorganic materials and surfaces will be influenced by the type, structure and property of the organic group(s) introduced by the organoalkoxysilanes. Our research groups develops new synthetic methods to rationally design bridge-bonded organoalkoxysilane precursors and/or self-assemble and co-assemble mixtures of organosilanes into multifunctional nanoporous organosilica and organosilica-titania materials containing two functional groups in close proximity. We also investigate the materials' tunable properties and broader potential applications for catalysis compared to existing bifunctional materials. In this talk, I will describe the latest results from our group on the self-assembly of various organosilanes into multifunctional nanomaterials and their catalysis properties in various catalytic chemical transformations.