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The copolymerizations of anhydride‐cured epoxy resin on fiberglass surfaces treated with a N‐methylaminopropyltrimethoxysilane coupling agent has been investigated using Fourier‐transform infrared spectroscopy. The structure of the interface of the silane and the resin in fiber‐reinforced composites is composed of copolymers of the epoxy resin with the organofunctionality of the deposited silanes. The number of interfacial bonds formed depends on the amount of silane coupling agent deposited on the fiberglass and the reaction conditions. The silane induces additional esterification and increases the curing density of the epoxy matrix near the fiber surface by about 5–10% relative to the bulk resin.