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Carbonized polymer dots (CPDs) have shown exceptional potential across a wide range of applications. However, their practical utilization is significantly greatly impeded by the lack of precise control over their structures and functionalities. Consequently, the development of controlled synthesis strategies for CPDs with well-defined structures and tailored functionalities remains a critical challenge in the field. Here, the controlled synthesis of functional CPDs with reversible assembly properties via airflow-assisted melt polymerization, followed by a one-step post-synthetic doping strategy, is reported. This synthetic approach achieves high product yield, uniform and tunable structures, as well as customized functionalities including solid-state emission, enhanced catalytic performance (3.5-45 times higher than conventional methods), and selective gas storage in the resulting CPDs. The ability to tailor the properties of CPDs through controlled synthesis opens up new opportunities for their practical application in photocatalysis and gas storage., (© 2024 The Author(s). Advanced Science published by Wiley‐VCH GmbH.)