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Ground‐level ozone (O3) and atmospheric fine particulate matter (PM2.5) pollution are the major challenges for continually improving air quality in the Yangtze River Delta (YRD) region of China. Understanding regional transport patterns of PM2.5 and O3 pollution is essential for the development of regional cooperative prevention strategies. This study shows the annual concentration of PM2.5 in the YRD decreased by 18.5% from 2015 to 2018, while the mean values of the daily maximum 8‐hr average (MDA8) O3 concentration from March to October increased by 16.3%. A complex network method is utilized to investigate the regional transport of PM2.5 and O3 in different grid cells (nodes). The source apportionment method within the chemistry transport model is applied to verify the reliability of the complex network method. Interregional and intraregional transport play an important role in both PM2.5 and O3 over the YRD. The northern part of the YRD contributes much more than other areas, while the central part of the YRD, especially the southern part of Jiangsu, is the largest contributor of O3 in the YRD in the summer, accounting for about 70%. Intraregional transport plays more of a major role in increasing PM2.5 pollution than O3 pollution. This study not only verifies the transport patterns of heavy pollution through the complex network method and traditional source apportionment technology, it also reveals that both methods provide great potential in understanding transport patterns and air pollution relationships, which are the solid foundation for emission mitigation in the YRD region. Key Points: Complex network method provides a foundation for an in‐depth analysis of regional transport with chemical transport model at grid levelThe results show that the Suxichang and Hangjiahu areas are the most prominent contributors of both PM2.5 and O3 in the Yangtze River Delta (YRD)The southern Huangshan and the border of Jinhua and Lishui are the major receptors for PM2.5 and O3 in the YRD [ABSTRACT FROM AUTHOR]