We report the synthesis and characterization of multiwalled carbon nanotube (MWCNT)– organically modified silicate (ORMOSIL) nanohybrid gel glass, in which the incorporated MWCNTs are covalently bonded to the silica network. The structural properties of the 3-aminopropyltriethoxysilane functionalized MWCNTs and MWCNT–ORMOSIL nanohybrid gel glass are comprehensively characterized using spectroscopic and electron microscopy techniques. We find that the agglomeration of incorporated MWCNTs is effectively restrained and that the MWCNTs are dispersed homogeneously and individually in the gel glass matrix. Compared with the mother MWCNT suspension, the resultant nanohybrid gel glasses demonstrate sustained nonlinear optical properties at both 532 and 1064 nm laser wavelengths.