In this study, bentonite clay was modified through silane treatment and calcination to enhance its compatibility with basalt fiber (BF) and epoxy in multiscale composites. The as-received bentonite (ARB) was subjected to silane treatment using APTES, producing silane-modified bentonite (STB), while calcination yielded calcined bentonite (CB). The modified clays were incorporated into basalt fiber-reinforced epoxy (BFRP) composites, which were fabricated using the vacuum-assisted resin transfer method (VARTM). Analytical techniques, including X-ray diffraction (XRD) and Fourier-transform infrared (FTIR) spectroscopy, confirmed the structural changes in the clays. BET surface area analysis revealed a 314% increase in the surface area of STB and a 176% increase for CB. The modified clays also demonstrated reduced hydrophilicity and swelling behavior. Thermogravimetric analysis (TGA) indicated a minimal improvement in thermal stability, with the degradation onset temperatures increasing by less than 3 °C. However, tensile tests showed significant gains, with CB- and STB-reinforced composites achieving 48% and 21% higher tensile strength than ARB-reinforced composites. Tribological tests revealed substantial reductions in wear, with CB- and STB-reinforced composites showing 90% and 84% decreases in the wear volume, respectively. These findings highlight the potential of modified bentonite clays to improve the mechanical and wear properties of basalt fiber–epoxy composites.