The essential objective of this work was to investigate the effect of silane treatment on the tensile and impact strength of composites made of jute/kenaf/glass fibers with the TiO2 nano-filler. This study also sought to optimize the factors connected with this treatment method. To develop and evaluate trials, the researchers used Response Surface Methodology (RSM) with central composite designs, emphasizing the optimization of silane concentration, immersion time, and nano-filler content. The researchers were able to effectively create quadratic models to forecast the tensile and impact strengths of the nano-composite throughout the silane treatment procedure. The adjustment of silane concentration, immersion duration, and nano-filler content discovered the best conditions for obtaining maximum tensile strength. The optimal values for silane concentration and immersion time have been identified to be 15 wt. % and 30 min, respectively. Considering these conditions, the composite’s tensile strength increased by 32.13% and its impact strength improved by 8.34% above the lowest values achieved from RSM optimization. The results demonstrate the practical value of silane treatment, notably in boosting tensile and impact strengths while enhancing interfacial adhesive among natural fibers and polymer matrices.