We study the voltage control of perpendicular magnetic anisotropy in an ultrathin Fe layer sandwiched between the Cr buffer and MgO tunneling barrier layers. A high-interface magnetic anisotropy energy of 2.1 mJ/m(2) is achieved in the Cr/ultrathin Fe/MgO structure. A large voltage-induced perpendicular magnetic anisotropy change is observed under the negative-bias voltage applications for the case of the Fe layer thinner than 0.6 nm. The amplitude of the voltage-induced anisotropy energy change exhibits a strong Fe-thickness dependence and it reaches as high as 290 fJ/Vm. The observed high values of the surface anisotropy and voltage-induced anisotropy energy change demonstrate the feasibility of voltage-driven spintronic devices.