Phospholipids comprise an enormous range of chemical structures that provide much of the functionality associated with cellular membranes. We have developed a simple method for incorporating phospholipids onto the surfaces of anisotropic gold nanorods as a stepping-stone for creating responsive and multifunctional nanocomposites. In this report, we demonstrate how phospholipids can be used to control the self-assembly of gold nanorods into agglomerate architectures ranging from open "end-to-end" networks to densely packed "side-to-side" arrays. The results indicate that lipid-gold nanorod assembly is governed by the tuning of electrostatic interactions within the phospholipid layers as well as by how the phospholipid layers organize themselves around anisotropic nanorod surfaces.