The essential function of biomembranes is to serve as barriers that compartmentalize cells and intracellular organelles from the external environment. They also provide functional interfaces responsible for intercellular communication, substance transport, and energy production. These complex functions are achieved through the dynamic formation of supramolecular assemblies of lipid bilayers and membrane proteins working in concert. Establishing methods to control the physical properties of lipid membranes and modulate their functions is indispensable for realizing molecular robotics using artificial cell membranes. In this chapter, we present examples of methods to control the properties and related functions of lipid membranes using engineered synthetic membrane-active polymers. Specifically, we designed and synthesized a series of amphiphilic polymers that mimic the membrane-binding motifs of natural proteins or peptides to induce pore formation in lipid membranes, lipid domain formation, and lipid nanodisc formation.