This work aims to contribute to a better understanding of the ionic strength effect on microcystin and natural organic matter (NOM) surrogate adsorption by analyzing the importance of adsorbate molecular size, and surface concentration. Adsorption kinetics and/or isotherms were performed on PAC Norit SA-UF for four microcystin variants (MC-LR, MC-LY, MC-LW, MC-LF), and three NOM surrogates (salicylic acid (SA), tannic acid (TA), Aldrich humic acid (AHA)) at different solution ionic strengths. Results showed that the ionic strength effect depends upon the adsorbate surface concentration, cation charge (mono or divalent), and adsorbate molecular size. Potassium seemed not to affect the MC-LR adsorption, while calcium enhanced MC-LR kinetics and adsorption capacity. K + and, particularly, Ca 2+ improved the adsorption kinetics of the other microcystin variants. For identical surface concentration and ionic strength, the impact of K + and Ca 2+ on NOM surrogates depended on the adsorbate molecular size: K + effect was only observed for AHA, whereas Ca 2+ caused no effect on SA adsorption, slightly enhanced TA adsorption, and greatly enhanced AHA adsorption. MC-LR isotherms with two salt concentrations (KCl or CaCl 2) indicated that, for the studied range of equilibrium surface concentration (5.3–18.7 mg/g), an enhanced adsorption regime prevails, and no transition regime was observed.