This paper aims to disclose the effects of surface modification on the morphological, thermal and mechanical properties of olive pomace flour (OPF) reinforced polystyrene composites. First, the OPF was treated by the silane coupling agent: 3-(Trimethoxysilyl) propyl methacrylate (TMSPMA). Then, the treated OPF was added to polystyrene (PS) at different ratios, creating the composite samples. The structural and property changes resulting from this treatment were observed and discussed through Fourier transform infrared spectroscopy (FTIR), morphological analysis, thermal analysis and mechanical analysis. The results show that, with the growing OPF content, the tensile strength and elongation at break of the composites decreased, while the Young's modulus increased; the composites prepared with the silane coupling agent were more thermally stable than the untreated composites; the filler-matrix interaction was improved through the surface modification of the OPF by the TMSPMA).