High performance silanized silica/epoxy nanocomposites were prepared through mixing epoxy, tetraethyl orthosilicate (TEOS), (3-aminopropyl)trimethoxysilane (APTMS) and ammonia solution at 50 C. This all-in-one "Solvent-Free One-Pot Synthesis" results in nanocomposites with uniform dispersion of oval shaped silica nanoparticles and strong adhesion between silica and epoxy matrix. The influence of the synthesis conditions, such as molar ratio of NH3:TEOS, aging time, curing process and silica content on the thermal mechanical properties of nanocomposites were studied. The silanized silica/epoxy nanocomposite prepared in this study exhibits better thermal mechanical property in comparison with neat epoxy, non-functionalized silica/epoxy and commercialized silica/epoxy systems. The prepared nanocomposite with 3 wt% silanized silica exhibits 20%, 17% and 6% improvements on flexural, tensile and storage modulus over those of neat epoxy, respectively. (C) 2010 Elsevier Ltd. All rights reserved.