The phospholipid molecule is a typical component of the cell membrane. In particular, the phosphorylcholine polar group is an electrically neutral head group. 2-Methacryloyloxyethyl phosphorylcholine (MPC) comprising a phosphorylcholine group side chain was designed with the cell membrane as an inspiration. Versatile polymers comprising MPC could be synthesized, and their specific biofunctions were evaluated. Establishing an ultimate biointerface with multiple functions is important from the viewpoint of biomaterials science. Nonspecific protein adsorption is essential for achieving versatile biomedical applications. Simultaneously, bioconjugation and retention of its biofunction are crucial for a high-performance biointerface. In this review article, a tunable biointerface comprising MPCs was introduced. In particular, the use of nanoparticles and polymer brushes as biointerfaces was described along with the perspective versatility of their biological applications.