Highly efficient lubricating boundary layers at biosurfaces such as cartilage have been proposed to comprise phospholipids complexed with biomacromolecules exposed at the surfaces. To gain insight into this, a systematic study on the normal and frictional forces between surfaces bearing a sequentially deposited model alginate-on-chitosan bilayer, bearing different adsorbed phosphatidylcholine (PC) liposomes, was carried out using a surface force balance. Structures of the resulting surface complexes were determined using atomic force microscopy (AFM) and cryo-scanning electron microscopy (cryo-SEM). The liposome/lipid-polymer complexes could maintain their integrity up to high pressures in terms of both normal and shear interactions between the surfaces, which were repeatable, reproducible, and revealed very low friction (coefficient of friction mu down to 10(-3)-10(-4), depending on the PC used) up to pressures of hundreds of atm. We attribute this remarkable lubrication capability ultimately to hydration lubrication acting at the hydrated phosphocholine headgroups of the PC lipids, either exposed at the liposome surfaces or through complexation with the polyelectrolyte bilayer. Values of mu, while low, were roughly an order of magnitude higher than for the same PC vesicles adsorbed on bare mica, a difference attributed to their lower density on the bilayer; the bilayer, however, stabilized the PC-vesicles far better than bare mica against rupture and shear at high compressions and sliding.