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For the protection of human and ecological receptors from the effects of soil pollution with chemical compounds, we need to know the behavior and transport of pollutants in soil. This work investigated the Congo red (CR) acid dye sorption on three natural soils collected from central and northeastern regions of Romania, symbolized as IS-65, IS-T, and MH-13. To define the mechanism of sorption and identify the rate governing step, various diffusion models such as Weber–Morris intraparticle diffusion, Boyd, film and pores diffusion, and mass transfer analysis have been verified. The intraparticle diffusion analysis of Congo red sorption onto soils has been described by a multi-linear plots, showing that the sorption process takes place by surface sorption and intraparticle diffusion in macro, meso, and micropores. The values of intraparticle diffusion coefficient k_id increased with any rise of the initial concentration of pollutant. The results show that the values of pore diffusion coefficient (D_p) and film diffusion coefficient (D_f) are found to be from 10⁻⁸ to 10⁻¹⁰ cm² s⁻¹, indicating that film diffusion influences the sorption rate limiting step. The intraparticle diffusion analysis shows that the plots did not pass through the origin and have two distinct parts, confirming that intraparticle diffusion is not the single determining mechanism involved in the sorption of Congo red on soils IS-65, IS-T, and MH-13. The results revealed that the sorption process has a complex nature, since both external diffusion and internal diffusion are involved in the sorption of CR from solution onto the investigated soils.