In this study, the pulsed field gradient (PFG) nuclear magnetic resonance (NMR) technique was used for the investigation of (1) concentration and compression effects on cation self-diffusion, and (2) restricted diffusion of cations in cartilage. Since physiologically relevant cations like Na+ are difficult to investigate owing to their very short relaxation times, the cations tetramethylammonium (TMA) and tetraethylammonium (TEA) were employed for diffusion studies in samples of explanted cartilage. Results indicated that the diffusion of monovalent cations shows strong similarities to observations already made in studies of the diffusion of water in cartilage: with increasing compression, i.e. decreasing water content, the diffusion coefficient of the cation decreases concomitantly. The diffusion coefficients also showed a decrease with increasing cation concentrations, basically reflecting the corresponding decrease in the water content. Both results could be explained by the well-established model of Mackie and Meares. This, together with the similarity of the diffusion coefficient D in cartilage relative to free solution (about 50%) for both cations, is consistent with the view that the water content and not the charge is the most important determinant of the intratissue diffusivity of monovalent cations. Diffusion studies with increasing observation times showed strong evidence of restricted diffusion, allowing the estimation of the geometry of barriers within cartilage.