Thermochromic smart windows can provide innovative energy savings via intelligently modulating the transmittance of indoor solar radiation to reduce the energy consumption of air conditioning in buildings. Vanadium dioxide (VO2) has desirable thermochromic properties and great prospects in smart windows. Herein, 3D ordered macroporous (3DOM) VO2 films are prepared via a sacrificial colloid template method. The as‐fabricated 3DOM VO2 films exhibit a pure monoclinic phase with a uniform layout, controllable thickness and domain sizes, and excellent optical properties. Compared to a nontemplated film, the 3DOM structured VO2 exhibits improved thermochromic performance with a high solar modulation ability (ΔTsol) of 10.8% and an ultrahigh visible transmittance (Tvis) of 71.1%. In the near‐infrared region, a large contrast transmittance of 59.5% at 2500 nm is obtained for the 3DOM VO2 film. Such excellent optical properties arising from the 3DOM structure are also demonstrated by finite element analysis. This work offers a promising way to manipulate the optical properties of a VO2 thermochromic film via structural engineering for the deployment of smart windows.
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