A two-phase method is exploited to prepare many kinds of nearly monodisperse, highly crystalline, size- and shape-controlled, surface-property-tunable inorganic nanocrystals, such as metal, semiconducting, magnetic, dielectric, and rare earth nanocrystals. The reaction of the two-phase system happens at the interface between the oil (nonpolar) and water (polar) phases and the interface is an exclusive site for both nucleation and growth. Interestingly, many solvent pairs with a clear interface can be applied to synthesize inorganic nanocrystals successfully. Generally, as-prepared nanocrystals with organic ligands are soluble in nonpolar solvents. Furthermore, exchange of ligands can also be realized readily and the final nanocrystals can be soluble in polar solvents. This two-phase method is a simple, reproducible, and general route and is becoming as powerful an approach as other solution-based synthetic approaches to high-quality inorganic nanocrystals.