1. 1. In contrast to egg phosphatidylcholine, aqueous dispersions of phosphatidylserine exist as a single lamellar liquid crystalline phase up to a water content of approx. 75% with all the water intercalated between the bilayers. In the absence of salt the lamellae of the large multilamelar particles present in dispersions ( c = (g lipid)/(g lipid + g water) > 0.2) are corrugated, particularly the outer lamellae. In the absence of salt planar phosphatidylserine bilayers are less stable than those of neutral phosphatidylcholine. 2. 2. At low lipid concentrations ( c < 0.05) the structural organisation is not yet clearly defined but theoretical X-ray scattering curves calculated for model particles suggest that no extensive multilamellar packing remains. 3. 3. Sonication of phosphatidylserine dispersions produces vesicles varying in size and surrounded by a closed, single bilayer in which the structural organisation of the fundamental lipid bilayer is maintained. In the absence of salt the average vesicle diameter is 16.5 mm (165 Å), about 7–10 nm (70–100 Å) smaller than the average diameter of phosphatidylcholine vesicles. In the presence of salt (0.1 M NaCl, 0.01 M Tris, pH 8.1) the average vesicle diameter is 25 nm (250 Å) identical with that of phosphatidylcholine vesicles. 4. 4. Reducing the double layer repulsion by adding NaCl to unsonicated dispersions ( c > 0.05) leads to the extrusion of water from the interbilayer space and a reduction in the lamellar repeat distance. The multilamellar particles shrink and their lamellae become smooth, indicative of an ordering in the packing of the lamellae. In dilute unsonicated dispersions ( c > 0.05) increasing the ionic strength increases the order and extent of the multilamellar structures. Increasing the ionic strength in sonicated dispersions containing single shelled vesicles leads to aggregation and/or coalescence producing larger single bilayer vesicles as well as multilamellar structures. 5. 5. Time-dependent structural changes in unsonicated phosphatidylserine dispersions in salt-free water are observed which are due to the reorganization of small multilamellar regions, randomly oriented with respect to each other, into more extensive and more ordered multilamellar regions. Aggregation and/or coalescence of single bilayer vesicles occurs in sonicated phosphatidylserine dispersions. This process is temperature dependent and increases with increasing temperature. The structures present in aqueous dispersions after preparation are not in thermodynamic equilibrium. 6. 6. Structural details derived from X-ray diffraction and electron micrographs of free-etched preparations of phosphatidylserine dispersions are consistent with each other. The negative-staining procedure, however, produces artifacts with dispersions of acidic phospholipids.