The adsorption performance of pyridine onto polyaluminium chloride (PAC) and anionic polyacrylamide (APAM) water treatment residuals (WTRs) was investigated by batch experiments. This study confirmed the assumption that PAC-APAM WTRs had the ability to remove pyridine. The non-linear Dubinin-Radushkevich model and non-linear Freundlich model better described the isotherms, indicating that the adsorption was a chemically controlled multilayer process. The pyridine adsorption rate was simultaneously controlled by external film diffusion and intraparticle diffusion. The adsorption of pyridine was an endothermic reaction with randomness increase. The pyridine adsorption decreased with pH increase. Pyridine removal was observed to be a linear increase from 6.16% to 96.18%, with the increase of dosage from 2.5 g/L to 15 g/L. The Langmuir maximum adsorption capacity was 3.605 mg/g while the theoretical isotherm saturation capacity was 9.823 mg/g. Therefore, PAC-APAM WTRs recycled into contaminated soils for remediation is expected to be an innovative alternative disposal method. More research is recommended in the future to identify detailed adsorption mechanisms and the most appropriate mixing ratio of PAC-APAM WTRs to contaminated soils under various climatic conditions.