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Epoxy-based composites containing silica modified by various silane coupling agents (SCAs) were prepared. The effect of the SCAs and the silica content on the thermal, mechanical properties, and fracture toughness of the nanocomposites was investigated. The particle size and dispersion state of the modified silica particles in the matrix were determined by transmission electron microscopy. The modification of silica with SCAs was verified by Fourier transform infrared spectroscopy. The specific tensile properties at ambient temperature (AT, 298 K) were compared with those at cryogenic (LT, 77 K) condition for silica content of 1−5 wt%. The effect of certain types of coupling agents on the thermal properties of the composites was also investigated. The Tg of all amino-silane-modified composites tended to be improved at low silica contents, while that of epoxy-silane-modified composites seemed to be enhanced further at high silica content. The tensile properties of the nanocomposites both at AT and LT tended to be enhanced at lower silica content, especially the failure strain. The fracture toughness (KIC) turned out to be better enhanced by coupling agents at LT. The difference of the toughening mechanism at AT and LT was examined according to the morphology of the fracture surfaces using the scanning electron microscopy.