In this study, a new approach was used to prepare polymer composites reinforced by both nanoparticles and continuous fibers. Carbon nanofibers were prebound onto glass fiber mats, and then unsaturated polyester composites were prepared by vacuum-assisted resin transfer molding. Mechanical and thermal properties of these composites were measured and compared with those of the composites synthesized by premixing carbon nanofibers with the polymer resin. Flexural strength and modulus of composites improved with the incorporation of nanoparticles. Specifically, the property improvement was higher in the case of the composites prepared by the new prebound method. It was also found that carbon nanofibers increased the glass transition temperature and reduced the thermal expansion coefficient of unsaturated polyester composites.