Gallium oxide (Ga2O3) with a wide bandgap is emerging as one of the most promising candidates for solar-blind photodetectors (SBPDs). However, the practical application of Ga2O3-based SBPDs is impeded by substantial defects-related leakage currents, sluggish response speed, and high-cost, making their practical applications face great challenges. Here, we proposed strategic films growth regulation and surface state engineering to grow high-quality yet economical β-Ga2O3 films, thereby achieving high-performance SBPDs. High-resolution transmission electron microscopy revealed the presence of high-quality films with an extremely regular arrangement of β-Ga2O3 (2‾01) planes. The full width at half maximum and root mean square roughness values are 0.07° and 0.716 nm, respectively. The β-Ga2O3 films demonstrated a significant reduction in VO concentrations after O2/N2 plasma treatment. This process can effectively minimize thermal damage to the sample surface while retaining highly reactive free radicals. The photocurrents of devices can be further enhanced, leading to a larger PDCRs of 8.6 × 107, through N2 plasma treatment. Moreover, the films effectually suppress the persistent photoconductivity effect with τr and τd values of 5.31/0.97 s and 0.49/0.87 s before and after N2 plasma treatment, respectively. We have demonstrated the influence mechanism of O2/N2 plasma treatment on photoelectronic performance. This study provides a practical approach to growing high-quality β-Ga2O3 films and preparing high-performance but low-cost Ga2O3-based SBPDs.