This paper reports an experimental investigation of the self-assembly of phospholipids (L-alpha-phosphatidylcholine-beta-oleoyl-gamma-palmitoyl (L-POPC), dipalmitoyl phosphatidylcholine (DPPC), and L-alpha-dilauroyl phosphatidylcholine (L-DLPC)) at interfaces between aqueous phases and the nematic liquid crystal (LC) 4'-pentyl-4-cyanobiphenyl. Stable planar interfaces between the aqueous phases and LCs were created by hosting the LCs within gold grids (square pores with widths of 283 mu m and depths of 20 mu m). At these interfaces, the presence and lateral organization of the phospholipids leads to interface-driven orientational. transitions within the LC. By doping the phospholipids with a fluorescently labeled lipid (Texas Red-1,2-dipalmitoyl-sn-glycero-3-phosphoethanolamine (TR-DPPE)), quantitative epifluorescence microscopy revealed the saturation coverage of phospholipid at the interface to be that of a monolayer with an areal density of similar to 49 +/- 8% relative to hydrated lipid bilayers. By adsorbing phospholipids to the aqueous-LC interface from either vesicles or mixed micelles of dodecyltrimethylammonium and phospholipid, control of the areal density of phospholipid from 42 +/-10 to 102 +/- 18% of saturation monolayer coverage was demonstrated. Fluorescence recovery after photobleaching (FRAP) experiments performed by using laser scanning confocal microscopy (LSCM) revealed the lateral mobility of fluorescently labeled DPPE in L-DLPC assembled at the interface with the liquid crystal to be (6 +/- 1) x 10(-12) m(2)/s for densely packed monolayers. Variation of the surface coverage and composition of phospholipid led to changes in lateral diffusivity between (0.2 +/- 0.1) x 10(-12) and (15 +/- 2) x 10(-12) m(2)/s. We also observed the phospholipid-laden interface to be compartmentalized by the gold grid, thus allowing for the creation of patterned arrays of phospholipids at the LC-aqueous interface.