Technetium has been identified as an element of interest for the safety assessment of a deep geological repository for used nuclear fuel. In this study, the sorption of Tc(IV) onto MX-80 bentonite, illite, and shale in ionic strength (I) 0.1–6 mol·kgw−1 (m) Na-Ca-Cl solutions at pHm = 4–9 and limestone at pHm = 5–9 was studied. Tc(IV) sorption on MX-80 increased with pHm from 4 to 6, reached the maximum at pHm = 6–7, and then gradually decreased with pHm from 7 to 9. Tc(IV) sorption on illite gradually increased with pHm from 4 to 7, and then decreased as pHm increased. The sorption properties of Tc(IV) on shale were quite similar to those on illite. Tc(IV) sorption on limestone slightly increased with pHm from 5 to 6 and then seemed to be constant at pHm = 6–9. Tc(IV) sorption on all four solids was independent of ionic strength (0.1–6 m). The 2 site protolysis non-electrostatic surface complexation and cation exchange model successfully simulated the sorption of Tc(IV) onto MX-80 and illite and the optimized values of surface complexation constants were estimated.