The use of a silane coupling agent (methacryloxypropyl-trichlorosilane) to improve the mechanical properties of steel fiber-reinforced acrylic bone cements was assessed. Changes to the tensile and fracture properties of bone cements reinforced with silane-coated or uncoated 316L stainless steel fibers of different aspect ratios were studied. Contact-angle measurements indicated that the coupling agent coats the metal surface through room temperature treatments in a short time (within 2 h). Push-out tests indicated that the interfacial shear strength of silane-coated 316L stainless steel rods is 141% higher than the uncoated rods. The elastic moduli, ultimate stresses, and fracture toughness of the silane-coated, steel fiber-reinforced bone cements are significantly higher than the bone cements reinforced with uncoated steel fibers. There were no differences in the tensile mechanical properties of the silane-coated or uncoated, steel fiber-reinforced cements after aging in a physiological saline solution, indicating that the bonding effectiveness is decreased by the intrusion of water at the metal-polymer interface. Because of possible biocompatibility issues with leaching of the silane coupling agent and no long-term mechanical benefit in simulated aging experiments, the use of these agents is not recommended for in vivo use.