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High‐efficiency photocatalysts based on metal‐organic frameworks (MOFs) are often limited by poor charge separation and slow charge‐transfer kinetics. Herein, a novel MOF photocatalyst is successfully constructed by encapsulating C60 into a nano‐sized zirconium‐based MOF, NU‐901. By virtue of host‐guest interactions and uneven charge distribution, a substantial electrostatic potential difference is set‐up in C60@NU‐901. The direct consequence is a robust built‐in electric field, which tends to be 10.7 times higher in C60@NU‐901 than that found in NU‐901. In the catalyst, photogenerated charge carriers are efficiently separated and transported to the surface. For example, photocatalytic hydrogen evolution reaches 22.3 mmol g−1 h−1 for C60@NU‐901, which is among the highest values for MOFs. Our concept of enhancing charge separation by harnessing host‐guest interactions constitutes a promising strategy to design photocatalysts for efficient solar‐to‐chemical energy conversion. [ABSTRACT FROM AUTHOR]