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Highlights Transition metal phosphates were first developed for the electrochromic application. The obtained NiHPO4·3H2O film achieves an ultra-large optical modulation of 90.8%, and the electrochromic mechanism is systematically elucidated using in situ and ex situ techniques. A large-area electrochromic smart window with 100 cm2 is constructed, which displays superior performances in regulating natural lighting and storing electrical charges.