Vanadium dioxide (VO2) has reversible metal‐to‐insulator phase transitions (MIT) under thermal stimuli, which is a traditional and widely studied material for thermochromic smart window applications. Current research interests in VO2 materials design focused on decreasing phase change temperature (τc), increasing both luminous transmittance (Tlum) and solar modulating ability (▵Tsol). This review focuses on strategies for improving the thermochromic properties of VO2, including elemental doping to composite materials, improving the solar energy modulation ability, ameliorating color, elevating phase change efficiency, increasing durability, and enhancing energy efficiency. The challenges and opportunities of VO2 nanoparticles‐based thermochromic smart windows are discussed in the outlook section.