The active control of the leading-edge (LE) separation on the suction surface of a stalled airfoil (NACA 0012) at a Reynolds number of 106 based on the chord length is investigated through a computational study. The actuator is a steady or unsteady jet located on the suction surface of the airfoil. Unsteady Reynolds-Averaged Navier–Stokes (URANS) equations are solved on hybrid meshes with the Spalart–Allmaras turbulence model. Simulations are used to characterize the effects of the steady and unsteady actuation on the separated flows for a large range of angle of attack (0 < α < 28 deg). Parametric studies are carried out in the actuator design-space to investigate the control effectiveness and robustness. An optimal actuator position, angle, and frequency for the stalled angle of attack α = 19 deg are found. A significant increase of the lift coefficient is obtained (+ 84% with respect to the uncontrolled reference flow), and the stall is delayed from angle of attack of 18 deg to more than 25 deg. The physical nonlinear coupling between the actuator position, velocity angle, and frequency is investigated. The critical influence of the actuator location relative to the separation location is emphasized.