With the aim to determine the influence of dominant interlayer cation on the sorption and diffusion properties of bentonite, diffusion experiments with Sr on the compacted homoionous Ca- and Na-forms of Czech natural Mg/Ca bentonite using the planar source method were performed. The bentonite was compacted to 1400 kg·m⁻³, and diffusion experiments lasted 1, 3 or 5 days. Two methods of apparent diffusion coefficient D_a determination based on the analytical solution of diffusion equation for ideal boundary conditions in a linear form were compared and applied. The determined D_a value for Ca-bentonite was 1.36 times higher than that for Na-bentonite sample. Values of K_d were determined in independent batch sorption experiments and were extrapolated for the conditions of compacted bentonite. In spite of this treatment, the use of K_d values determined by batch sorption experiments on a loose material for the determination of effective diffusion coefficient D_e values from planar source diffusion experiments proved to be inconsistent with the standard Fickian description of diffusion taking into account only the pore diffusion in compacted bentonite. Discrepancies between K_d and D_e values were measured in independent experiments, and those that resulted from the evaluation of planar source diffusion experiments could be well explained by the phenomenon of surface diffusion. The obtained values of surface diffusion coefficients D_s were similar for both studied systems, and the predicted value of total effective diffusion coefficient D_e(tot) describing Sr transport in the Na-bentonite was four times higher than in the Ca-bentonite.