AbstractAs an important category of porous crystalline materials, metal‐organic frameworks (MOFs) have attracted extensive research interests owing to their unique structural features such as tunable pore structure and enormous surface area. Besides controlling the size, dimensionality, and composition of MOFs, further exploring the crystal‐phase‐dependent physicochemical properties is essential to improve their performances in various applications. Recently, great progress has been achieved in the phase engineering of nanomaterials (PEN), which provides an effective strategy to tune the functional properties of nanomaterials by modulating the arrangement of atoms. In this review, we adopt “phase” instead of “topology” to describe the crystal structure of MOFs and summarize the recent advances in phase engineering of MOFs. The two main strategies used to control the phase of MOFs, that is, phase‐controlled synthesis and phase transformation of MOFs, will be highlighted. The roles of various reaction parameters in controlling the crystal phase of MOFs are discussed. Then, the phase dependence of MOFs in various applications including luminescence, adsorption, and catalysis are introduced. Finally, some personal perspectives about the challenges and opportunities in this emerging field are presented.