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Photoenzymatic catalysis is an efficient strategy for selectively converting CO 2 into valuable chemicals. However, the sluggish reaction kinetics, resulting from low visible light utilization and rapid recombination of photogenerated carriers, severely inhibit the yields of target products. Herein, we present a novel artificial photosynthesis platform of 2D/2D MXene/crystalline COF-367 heterostructure for efficient conversion of CO 2 into HCOOH. This platform is extremely sensitive to solar light (λ ≤ 750 nm), with rapid charge separation and transfer due to the well-designed abundant ultrathin 2D/2D hetero-interfaces. Remarkably, Ti 3 C 2 /COF-367 achieves an impressive yield of 83.38% for coenzyme NADH regeneration with absence of electron mediator. Furthermore, it demonstrates a cascade ultra-high production rate of HCOOH at 1.88 mmol g−1 h−1 with almost 100 % selectivity. This work represents the first example of MXene to promote charge transfer in COFs-based photoenzymatic synergistic catalytic system, and provides insights into the development of organic/inorganic hybrids for CO 2 photoreduction. [Display omitted] • First example of MXene to promote charge transfer in COFs-based photoenzymatic catalytic system. • Ultrathin highly crystalline imine-linked COF-367 nanosheets were synthesized. • Abundant ultrathin 2D/2D hetero-interfaces for rapid charge separation/transfer. • Impressive NADH regeneration yield of 83.38% without electron mediator. • Ultra-high HCOOH production rate of 1.88 mmol g−1 h−1 with high selectivity. [ABSTRACT FROM AUTHOR]