The effects of ammonia-treated graphene oxide (GO) on composites based on epoxy resin were investigated. Ammonia solutions of different concentrations (14–28%) were used to modify GO. Nitrogen functional groups were introduced on the GO surfaces without significant structural changes. The ammonia-treated GO-based epoxy composites exhibited interesting changes in their mechanical properties related to the presence of nitrogen functional groups, particularly amine (C-NH2) groups on the GO surfaces. The highest tensile and impact strength values were 42.1 MPa and 12.3 J/m, respectively, which were observed in an epoxy composite prepared with GO treated with a 28% ammonia solution. This improved tensile strength was 2.2 and 1.3 times higher than those of the neat epoxy and the non-treated GO-based epoxy composite, respectively. The amine groups on the GO ensure its participation in the cross-linking reaction of the epoxy resin under amine curing agent condition and enhance its interfacial bonding with the epoxy resin.