Cesium lead halide perovskite nanocrystals (PNCs) have great potential in the field of lighting and display due to their excellent optical properties. The preparation of high-quality PNCs has always been the focus of scientific research. Herein, we present a facile two-phase method to synthesize high-quality CsPbBr3 nanoparticles. Both toluene and water served as reaction media and oleic acid as a strong bonding ligand was employed to synthesize the CsPbBr3 PNCs. High-quality CsPbBr3 PNCs with good crystallinity, narrow size distributions, and well surface passivation have been synthesized successfully. This study offers an alternative strategy for the preparation of high-quality perovskite materials.