Due to environmental concerns and budgetary constraints associated with synthetic fibers, natural fibers (NFr) are becoming increasingly popular as reinforcement in polymer composites (PCs) for structural components and construction materials. The surface treatment (ST) method is a well-established technique for enhancing the strength of interfacial bonding between NFr and the polymer matrix (PM). As a result, this research aims to determine the effect of ST with zinc oxide nanoparticles (ZnONPs) on the flexural properties of unsaturated polyester (UPE)/kenaf fiber (KF) nanocomposites. The hand lay-up technique was employed to produce KF-reinforced unsaturated polyester composites (KF/UPE) for this investigation. UPE/KF-ZnONPs composites were made with varying NFr loadings (weight percent), ranging from 10 to 40%. KF was treated with five distinct amounts of ZnONPs (from 1 to 5% weight percent). According to the findings of the investigation, the composite samples incorporating ZnONPs displayed superior optimum flexural properties compared to the untreated KF composite. It was found that 2% ZnONPs was optimal, and ST with ZnONPs could produce robust KF with improved flexural properties.