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This study is the first to propose the deployment of direct air capture (DAC) systems at large airports to provide solutions for achieving carbon neutrality in aviation transportation. Here, an estimating model for carbon dioxide (CO2) emissions in the landing and take-off (LTO) phase of large airports was developed, and the suitability of deploying DAC systems at airports was evaluated by the analytic hierarchy process (AHP). This study found that the annual CO2 emissions of 52 large airports in the LTO phase are about 23 Mt, accounting for about 23% of the total CO2 emissions of civil aviation in China. The four dimensions of airport transportation conditions, meteorological conditions, space resources, and security levels had a decreasing impact on the deployment of DAC systems in that order. The airports with suitable DAC systems are mainly located in the Yangtze River Delta, the Pearl River Delta, and the Chengdu-Chongqing Airport Cluster. This study provides a theoretical basis for the deployment of DAC systems at airports, which provides new CO2 emission reduction solutions for the aviation transportation industry. [ABSTRACT FROM AUTHOR]