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The environmental behavior of microplastics (MPs) has attracted global attention. Research has confirmed that MPs can strongly absorb almost every kind of pollutant and can serve as vectors for pollutant transport. In this research, the sorption isotherms of six organic pollutants with different structure on four virgin plastic particles with different crystallinity were determined. Results indicated that the hydrophobicity (K OW ) of organic pollutants and the crystallinity of MPs were the two key factors that affected the sorption process of organic pollutants on MPs. Strong correlations were observed between K OW and the partition coefficient. Hydrophobic partition was one of the major mechanisms regardless of the type of organic chemical (hydrophobic, polar, or dissociable). What is more, the influence of the crystallinity of MPs on the sorption process increased with increasing hydrophobicity of the chemical. Combining this result with analyzing the related literature on the effect of crystallinity, it was concluded that the effect of crystallinity on the sorption of chemicals with strong hydrophobicity was obvious, whereas this effect was negligible for chemicals with weak hydrophobicity. The influence of the crystallinity of MPs on sorption could even exceed the influence of MPs type, so crystallinity should be considered carefully when discussing the sorption capacity of MPs. This study enhances the understanding of the sorption of organic pollutants by MPs., (© 2024. The Author(s), under exclusive licence to Springer-Verlag GmbH Germany, part of Springer Nature.)