Local composition, structure, morphology, and phase are interrelated in lipid bilayer membranes. This work describes proofs-of-concept for methods that may be used and combined to modulate, to measure, and to probe the local structure of model membranes through control of membrane curvature in liposomes. These studies are performed using combinations of simultaneous two-color widefield fluorescence imaging, three-dimensional rendering of vesicle domains, and manipulation of the vesicle morphology via micropipet aspiration and the polymerization of cytoskeletal elements inside the membrane. Additionally, we report an electroformation method for preparing unilamellar lipid vesicles that allows hydration of membranes in physiological buffer conditions and formation of multicomponent/multiphase vesicles.