| Summary: | H<sub>2</sub> has aroused significant attention as an unpolluted and renewable energy carrier. However, the efficient storage and controllable release of H<sub>2</sub> are urgent to be addressed. Through the hydrogenation of CO<sub>2</sub> (bicarbonate) to produce formic acid (formate) and reverse dehydrogenation reactions, a carbon-neutral formic acid-based hydrogen cycle system can be established. Given the excellent recyclability and facile separation of heterogeneous catalysis, the development of heterogeneous catalysts for these reversible interconversions is thoroughly summarized, with a special focus on the structure–activity relationship and the mechanistic insight. Finally, the challenges and opportunities surrounding the formic acid-based hydrogen cycle system are discussed. It is hoped that this review will provide guidance and an idea for the design and development of efficient heterogeneous catalysts for the carbon-neutral H<sub>2</sub> storage and release system.
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