Plasma membranes are essential to the function of cellular systems. As a consequence of this fact many proteins and other biological species are not active outside of their native environment. It would be ideal to create an artificial structure that could house selected biomolecules in their active forms, enabling their use in applications such as bio-sensing, for example. As the understanding of these complex and dynamic bilayer structures increases, it has become clear that their stability in air is not sufficient for use in many chemical sensing applications. For this reason, the work presented here was undertaken to find ways to optimize interactions between lipids and planar substrates, enabling the formation of air-stable lipid adlayers. Several phospholipids were explored; 1,2-dimyristoyl-sn-glycero-3-phosphatidic acid (DMPA), 1,2-dimyristoyl-sn-glycero-3-phosphocholine (DMPC), 1,2-dimyristoyl-sn-glycero-3-phosphoethanolamine (DMPE), 1,2-dimyristoyl-sn-glycero-3-[phospho-rac-(1-glycerol)] (DMPG), and 1,2-dimyristoyl-sn-glycero-3-[phospho-L-serine] (DMPS). These lipids, in vesicle form, were exposed to chemically modified substrates and underwent vesicle fusion to create lipid adlayers. The Au substrates on which the adlayers were deposited were modified to interact with the phospholipid headgroups. The resulting lipid adlayer was stable with respect to transport across the water/air boundary. The chemical modification of the interface was accomplished using 6-mercapto-1-hexanol to form a self-assembled monolayer characterized by a polar, hydrophilic interface. The 6-mercapto-1-hexanol monolayer was reacted with POC1₃ and water to create a phosphate-terminated interface. The phosphate functionalities were populated with Zr⁴⁺ ions, rendering them capable of complexation with phospholipid phosphate moieties. Other metal salts were also used to gain insight into the effect of metal ion identity on the binding of phospholipids. To characterize the lipid adlayers, time correlated ellipsometry, water contact angle, cyclic voltametery, XPS, ³¹P-NMR and FTIR measurements where used. All of the analyses performed were ex-situ from the lipid deposition vessel, demonstrating air-stable adlayer formation. Each technique interrogated a different adlayer property. The discovery of a novel family of self-assembling adlayer comprised of biologically important molecules opens the possibility of future success in the creation of robust biomimetic interfacial structures.