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Solar‐driven CO2 conversion to fuels is a central technique for closing the anthropogenic carbon cycle, but to date is limited by the intermittent solar flux. To face this challenge, a catalyst is needed that can work well in both light and dark. Here, surface oxygen vacancies are created in a Sr2MgSi2O7:Eu2+,Dy3+ long‐afterglow phosphor with long‐time and high charge storage capacity (denoted as...