The main objective of the present work was to study the effects of nano-TiO2 on the dry-sliding wear properties and interlaminar shear strength of jute fiber/epoxy composite. The surface of TiO2 nanoparticles was functionalized by using a amin-terminated silane-coupling agent. Fourier-transform infrared spectroscopy and thermogravimetric analysis were used to characterize the modified TiO2 (M-TiO2). The multiscale composites were fabricated using hand layup technique by dispersing various amounts of the M-TiO2 nanoparticles (0.5, 1, 3, and 5 wt.%) in the matrix. Among these specimens, the 3 wt.% M-TiO2-filled composite showed the best properties. The results of the short-beam shear test demonstrated that the addition of 3 wt.% M-TiO2 increased the interlaminar shear strength of the composite by 43%. The addition of 3 wt.% M-TiO2 significantly decreased the wear rate and coefficient of friction of the jute fiber/epoxy composite by 80% and 48%, respectively. The wear and fracture mechanisam were also examined by scanning electron microscopy. The findings of this work confirmed that the addition M-TiO2 is a suitable choice for the potential applicability as a nanofiller for the fiber-reinforced polymeric composites.