The lipid content and composition of these pellicles and the effect of lipids on their ability to retard the diffusion of lactic acid were investigated. Lipids accounted for 22.4% of the dry weight of caries-resistant enamel pellicle and 19.2% of caries-resistant cementum pellicle; the pellicle of caries-susceptible enamel contained 24.6% lipids and that of caries-susceptible cementum, 23.4%. Enamel and cementum pellicles from caries-resistant saliva had a significantly lower content of neutral lipids and phospholipids, whereas the glycolipid content was lower, although not significantly, in caries-susceptible pellicles. Pellicles from caries-resistant saliva had a considerably greater capacity to retard lactic acid diffusion than those from caries-susceptible saliva. In all cases, the retardation capacity was clearly dependent upon the lipid constituents, removal of which caused a 50-52% drop in lactic acid impedance by caries-resistant enamel and cementum pellicles, and 32-35% drop by caries-susceptible pellicles. On reacting the delipidated pellicles with their lipids, it was found that, in all cases, the highest quantitative effect on the restoration of the retardation capacity occurred when phospholipids were added. The findings suggest that the events controlling the interaction of salivary phospholipids with enamel and cementum may determine the susceptibility of the tooth surface to demineralization by acids produced by cariogenic micro-organisms.