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To enhance the flexural properties of glass fiber‐reinforced vinyl ester resin (GF‐VER) composites, this study focused on the influence of the duration of surface treatment on the flexural properties using polydopamine (PDA) and nanosilicon dioxide (nano‐SiO2). The GF‐VER composites were prepared via hot pressing. Fourier transform infrared spectroscopy (FTIR) and scanning electron microscopy (SEM) were utilized to characterize the microstructural and chemical attributes of the GF and GF‐VER composites. The mechanical properties of the GF‐VER composites were characterized using the flexural strength test. Furthermore, thermogravimetry was employed to investigate the thermal stability of the GF and the content of PDA nanoparticles on the GF. The results demonstrated that upon extending the treatment period, a greater quantity of PDA‐SiO2 nanoparticles adhered to the surface of the GF. The analysis of these results established that the optimal treatment duration is 12 h. This duration facilitated an enhanced adhesion between GF and VER owing to PDA‐SiO2, resulting in an optimal flexural strength of 562.8 MPa and signifying a 8.86% increase compared with the flexural strength of the untreated GF‐VER composites. Overall, the findings indicate that PDA‐SiO2 treatment greatly improves the flexural strength of GF‐VER composites. Highlights: The method for modifying the GF surface was simple and mild.Silica nanoparticles were grafted onto GFs using dopamine as a reaction platform.The effect of the duration of PDA‐SiO2 treatment on the flexural strength of GF‐VER composites was examined.SEM revealed an improved GF‐VER interface.The flexural strength of the GF‐VER composites improved by 8.86%. [ABSTRACT FROM AUTHOR]