LAUSR

Li‐O2 batteries have attracted extensive attention because of their theoretical specific energy equivalent to gasoline, but the poor electrical conductivity of Li2O2 leads to high overpotential, which limits their further development and application. Herein, this work introduces Ce‐UiO‐66, a metal‐organic framework material, as the photocatalyst to reduce the overpotential in the discharging and charging processes. With the simple in situ growth of Ce‐UiO‐66 on carbon cloth as an integrated photocathode, the photoassisted Li‐O2 batteries display decent discharge and charge voltages of 3.1 and 3.6 V, and a lifespan of 160 cycles. Moreover, theoretical calculations have been carried out to understand the band structure, spectroscopy, and photocatalytic property of Ce‐UiO‐66. The findings will encourage an enormous variety of novel MOFs‐based photocathodes for solar energy utilization systems.