In the past decade extensive studies have been focused on mechanical properties of inorganic nanofiller/epoxy matrices. In this work we systematically investigated the mechanical properties of nano-alumina-filled E-54/4, 4-diaminodiphenylsulphone (DDS) epoxy resins, which were prepared via combining high-speed mixing with three-roll milling. Homogeneous dispersion of nano-alumina with small agglomerates was obtained in epoxy resin, which was confirmed using transmission electron microscopy (TEM). The static/dynamic modulus, tensile strength and fracture toughness of the nanocomposites were found to be simultaneously enhanced with addition of nano-alumina fillers. About 50% and 80% increases of K(IC) and G(IC) were achieved in nanocomposite filled with 18.4 wt% alumina nanofillers, as compared to that of the unfilled epoxy resin. Furthermore, the corresponding fracture surfaces of tensile and compact tension samples were examined by scanning electron microscopy (SEM) and atomic force microscopy (AFM) techniques in order to identify the relevant fracture mechanisms involved. Various fracture features including cavities/debonding of nanofiller, local plastic deformation as well as crack pinning/deflection were found to be operative in the presence of nano-alumina fillers.