SUMMARYThe crystallization behaviour of bilayers of synthetic phosphatidylcholines in the presence of cholesterol was investigated by freeze fracturing.I. Below the lipid-phase transition, cholesterol is randomly distributed over the lateral plane of a bilayer of the single species dimyristoylphosphatidylcholine, as far as can be detected within the lateral resolution of freeze fracturing.2. in an equimolar mixture of dilauroyl-and dimyristoylphosphatidylcholine, which shows cocrystallization, cholesterol is distributed randomly in the bilayers below the phase-transition temperature.3. In an equimolar mixture of dipalmitoyl and l-palmitoyl-2-oleoylphosphatidylcholine, which shows monotectic behaviour, cholesterol interacts preferentially with the liquid crystalline species 1-palmitoyl-2-oleoylphosphatidylcholine when the other component dipalmitoylphosphatidylcholine passes from the liquid crystalline to the gel state upon cooling the mixture.