In order to improve the mechanical and bond properties of epoxy adhesives for their wide scope of applications, modified epoxy adhesives were produced in this study with SiO2 nanoparticles of 20 nm in size, including inactive groups, NH2 active groups, and C4H8 active groups. The mechanical properties of specimens were examined, and an investigation was conducted into the effects of epoxy adhesive modified by three kinds of SiO2 nanoparticles on the bond properties of carbon fiber reinforced polymer and steel (CFRP/steel) double lap joints. According to scanning electron microscopy (SEM), the distribution effect in epoxy adhesive of SiO2 nanoparticles modified by active groups was better than that of inactive groups. When the mass fraction of SiO2-C4H8 nanoparticles was 0.05%, the tensile strength, tensile modulus, elongation at break, bending strength, flexural modulus, and impact strength of the epoxy adhesives reached their maximum, which were 47.63%, 44.81%, 57.31%, 62.17%, 33.72%, 78.89%, and 68.86% higher than that of the EP, respectively, and 8.45%, 9.52%, 9.24%, 20.22%, 17.76%, 20.18%, and 12.65% higher than that of the inactive groups of SiO2 nanoparticles, respectively. The SiO2 nanoparticles modified with NH2 or C4H8 active groups were effective in improving the ultimate load-bearing capacity and bond properties of epoxy adhesives glued to CFRP/steel double lap joints, thus increasing the strain and interface shear stress peak value of the CFRP surface.