Constructing heterostructured photocatalysts is an efficient method to improve photocatalytic carbon dioxide (CO2) reduction. Herein, holey g-C3N4 (HGN) with rich amino groups (−NH x ) was hybridized with NH2-UiO-66 (NUZ) via a facile in situ growth method. NUZ nanocrystals were anchored on HGN via NHx–Zr–O chemical bonding, leading to the uniform dispersion and avoiding the leaching of NUZ, thus showing excellent stability in photocatalysis. The chemically bonded interfacial charge transfer effect originated from the NHx–Zr–O formation efficiently accelerated the separation and migration of charge carriers, improving the photoactivity. Benefiting from the NHx–Zr–O formation, the optimized NUZ/HGN-35% heterojunctions exhibited outstanding activity in the photoreduction of CO2 to CO (31.6 μmol g–1 h–1), which was about 2 and 3 times higher than that of pure NUZ and HGN under visible-light irradiation. This study is expected to provide useful insights for constructing composites with strong interaction for CO2 reduction, H2 production, and N2 reduction.