The gas–liquid Venturi injector has been widely applied in industrial production due to its advantages of high entrainment and low energy consumption. In this study, Computational Fluid Dynamics (CFD) was employed to investigate the effect of the gas–liquid interface structure within the mixing section on entrainment behavior by varying the geometry of the mixing section during gas–liquid coaxial flow. The simulation results indicate that along the jet direction, the gas–liquid interface generally transitions from a smooth cylindrical shape to a lobed structure in the mixing section. Surface waves mainly appear in the lobed region. Furthermore, lobed and surface wave structures reduce pressure loss and enhance entrainment. Additionally, the study found that longer mixing sections enhance entrainment under low flow resistance. This study provides valuable insights for achieving high jet entrainment and offers supplementary research on gas–liquid interface structures in jets constrained by solid boundaries.