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For the efficient utilization of CO2 into valuable product, the attractive carbon nitride catalysts have been widely studied. In this work, heptazine‐related materials with varying degree of polymerization were designed by an intrinsically modification strategy and employed in the cycloaddition of CO2 with the bisepoxide 1, 4‐butanediol diglycidyl ether (BDODGE). We initially figured out that the sample prepared at 450 °C contained more melem hydrate, exhibiting the best performance. The epoxides conversion and corresponding cyclic carbonates selectivity could achieve 93.1 % and 99.3 % at 140 °C for 20 h without any cocatalyst and solvent, respectively. Results of the catalytic tests suggested that the high catalytic activity was dependent on big size porous structure and the synergetic effect of active amino groups and −OH groups. The role of water in maintaining the specific structure and providing active site has been proved. Moreover, the CN‐450‐W catalyst exhibited outstanding recycling stability. And finally, a plausible reaction mechanism was proposed. [ABSTRACT FROM AUTHOR]