alpha-Amino acid-beta-hydroxysiloxanes prepared previously by our group were coupled to E-glass fibers to gain a better understanding of the surface processes at the polymer-glass interface of composite materials. Use of DRIFT (diffuse reflectance infrared Fourier transform spectroscopy), XPS (X-ray photoelectron spectroscopy), and SEM techniques allowed for the qualitative and quantitative determination of such processes. Our studies indicate that binding to the E-glass is occurring through different mechanisms, primarily hydrogen bonding, as evidenced by DRIFT and SEM. XPS studies confirm that the amino group is binding to the surface, as evidenced by the formation of two amino states, a covalent nonprotonated and an ionic protonated form. A theoretical model depicting the binding of polymer to E-glass fibers has also been proposed.