In this paper, the Taguchi method with an L₉(3⁴) orthogonal array was used as experimental design to determine the optimum conditions for preparing ZnO nanoparticles via a mechanothermal route. ZnSO₄·H₂O and Na₂CO₃ were used as starting materials. The effects of milling time, Na₂CO₃/ZnSO₄·H₂O molar ratio, and ball-to-powder mass ratio (BPR) on the bandgap (E_g) of ZnO nanoparticles were investigated. The ranges of the investigated experimental conditions were 5–15 h for the milling time (t), 1.0–1.2 for the Na₂CO₃/ZnSO₄·H₂O molar ratio (M), and 10–30 for BPR. The milling time and BPR exhibited significant effects; an increase in milling time reduced the bandgap. The optimum conditions from this study were t₃ = 15 h, M₁ = 1, and BPR₂ = 20. Only two significant factors (t₃, 15 h; BPR₂, 20) were used to estimate the performance at the optimum conditions. The calculated bandgap was 3.12 eV, in reasonable agreement with the experimental results obtained under the optimized conditions.