The sneak path problem is one of the major hindrances to the application of high-density crossbar resistive random access memory; however, complementary resistive switching (CRS) is an effective solution to this problem. The co-existence of resistive switching (RS) and CRS is possible within the same device. Therefore, a precise control is highly required for the successful utilization of different modes. In this study, we have demonstrated an effective way to control both switching modes in a simple HfO2-based crossbar device. The interchange between RS and CRS modes is possible, based on the intrinsic anionic rearrangement by controlling the extrinsic stimulation, either in the form of voltage or in the form of current. In particular, a highly nonlinear CRS mode is reported, in which the nonlinearity is almost 100 times greater than in the RS mode, which is achieved at a high temperature of 150 °C. The procedure reported in this study may be useful for the other resistive memory systems.