To investigate the occurrence, gas–particle partitioning, and potential sources of polybrominated diphenyl ethers (PBDEs) in the atmosphere over the Yangtze River Estuary, gas and particle samples were collected at the remote Huaniao Island, East China Sea, during a whole year from 2013 to 2014. Nine PBDEs, with total atmospheric concentration of Σ₉BDEs of 20.3 ± 26.5 pg/m³, were found in both the gas and particle phases in most samples. BDE-209 dominated both the gas and particle phases, which is consistent with the PBDE usage record in China. Seasonal variation of particle-phase Σ₉BDEs was observed, with the highest concentration in winter and the lowest in summer; however, a reversed seasonal trend was observed in the gas phase. Correlation analysis between log K_p and log K_OA suggested that the gas–particle (G/P) partitioning was in a non-equilibrium state, particularly for BDE-209 throughout the year. The K_OA-based adsorption model prediction performed relatively well for the particle-phase fraction of Br_<10-BDEs, but largely overestimated BDE-209. A steady-state model could be superior to predict G/P partitioning of BDE-209 based on annual values, though with the exception of summer samples. A relatively higher gas-phase distribution for BDE-209 than high-brominated BDEs was observed, especially in summer, when it reached 73%, implying a sustained input of gas-phase BDE-209. The potential source contribution function showed that the possible source regions for BDE-209 included Shandong and Jiangsu Provinces (the main BDE-209 production regions in China), the Yangtze River Delta region, and the southeastern coastal areas (which hosts intensive electronic waste recycling activities).