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Smart windows with excellent near-infrared (NIR) light shielding capacity and controlled visible light transmittance are expected to reduce building energy consumption and improve indoor comfort. However, the ability of current thermochromic materials to regulate solar gain with the tunable extinction of phase-change materials is still far from optimum. In this work, an fluorine (F)-doped ATO (FATO) nanocrystals (NCs) are designed as a photothermal material to optimize the solar modulation of thermochromic hydrogels. F ion doping can modify the electronic structure of ATO, resulting in a high concentration of oxygen vacancies and free electrons, thereby enhancing the NIR absorption performance and photothermal conversion performance of the ATO NCs. On this premise, the designed smart window based on FATO NCs and thermochromic hydrogels exhibits the remarkable features of excellent NIR shielding, high initial visible transmittance and fast response speed. The window is capable of shielding 99.5% of the solar radiation from 300 to 2500 nm and permitting 75.0% of initial visible light. Moreover, the simulated indoor temperature of the smart window was 17.2 °C lower compared with the black one, demonstrating potentials in practical application of building energy saving. [Display omitted] • Novel chain-like FATO NCs were prepared by precipitation-hydrothermal method. • F-doping optimized electronic structure of ATO and improved the LSPR absorption. • The fabrication of FATO-PNC hydrogel provides a novel idea for smart window. • The smart window could shield 99.5% of solar radiation after optical switching. [ABSTRACT FROM AUTHOR]