Organic matter blocks highly selective frayed edge sites on clay minerals and reduces radiocaesium adsorption. The effects of different soil organic matter on Cs adsorption on illite have been investigated. The quantity and quality of soil organic matter was varied by extracting from three contrasting soils and varying extraction conditions. Extracted organic matter was quantified, and analysed using UV and fluorescent spectroscopy. Cs adsorption was markedly lower in soil aqueous extracts, than in simple electrolyte solution at the same ionic strength (IS). Part of the decrease was attributed to soluble soil potassium. After correction for ionic strength and potassium, the relative distribution coefficient of Cs, KdIS,K, decreased with increasing dissolved organic carbon (DOC) concentration. The correlation between KdIS,K and DOC was largely unchanged by taking into account any of the measured spectral parameters. We find no evidence that molecular size and composition of organic coatings determine their effect on the Cs adsorption properties of illite.