The superior mechanical flexibility, mechanical strength, electrical conductivity, high specific surface area, and a special two-dimensional crystalline structure make graphene a very promising building block material for flexible electromechanical actuators. However, graphene papers have exhibited limited electromechanical actuation strain in aqueous electrolyte solution. In this paper, we show an easy approach to significantly improve the electromechanical actuation of reduced graphene oxide (rGO) papers via fine tuning the oxygen functional groups in rGO sheets, which was achieved by careful control of quantity of the reduction agent used in the chemical reduction process of graphene oxide. The actuation strains are enhanced up to 0.2% at an applied voltage of 1 V, which is more than a 2 fold increase compared to the regular pristine rGO paper. Further theoretical and experimental analyses reveal that the change of the capacitance and the stiffness of the rGO papers are two key factors responsible for the observed improvement.