The effects of oxygen plasma treatment on the surface chemistry of Spectra 1000(R) high modulus polyethylene fibers and on the mechanical properties of fiber-reinforced composites of the fibers in a Bis-GMA based acrylic resin have been studied. X-ray photoelectron spectroscopy and diffuse reflectance FTIR spectroscopy have been used to show that the majority of oxygen on the fiber surface exists mostly in the form of ether and/or epoxy linkages, with carbonyl-, carboxylic- and ester-containing compounds accounting for less than 10 percent of the total. While the untreated and plasma-treated fibers have similar chemical compositions, the surfaces of the plasma-treated fibers are more polar and the oxygen is chemically bonded instead of being merely physisorbed. The interfacial shear strength between the fibers and the acrylic resin is increased by a factor of 2.3 by the plasma treatment indicating the presence of a weak boundary layer on the surface of the untreated fibers. The hydrolytic stability of the composite interfaces was investigated for fibers sized with several Bis-GMA-based adhesives. Maximum stability was attained by sizing with Bis-GMA containing a peroxide catalyst or an amine accelerator. The flexural properties of composites utilizing plasma-treated and untreated fibers were compared in three-point bending. The ultimate bending loads for composites using treated fibers were much higher than those for composites with untreated fibers, but only a fraction of that for glass or Kevlar(R)-reinforced materials.