Structure-property studies were carried out on a number of different hybrid sol·gel materials. Multifunctional silicon ethoxides were prepared and studied by solid state ²⁹Si NMR and Raman spectroscopy to determine the type of silicate structures formed and the degree of conversion attained by the sol-gel process under previously established reaction conditions. New procedures were developed to incorporate titaniumisopropoxide as well as Al, Zr and Zn acetylacetonates into functlonalized polyltetramethylene oxide) modified sol-gel systems. The physical properties of titanium containing poIy(tetramethyIene oxide) modified sol-gel materials were studied in detail and correlated to morphological and structural information gained from dynamic mechanical analysis, small angle x-ray scattering and scanning electron microscopy. The incorporation of titanium was found to increase the measured Young’s modulus and stress at break relative to comparable materials based solely on TEOS.