Revealing the nature of interaction between graphene oxide (GO) and lipid membrane is a crucial issue but still remains challenging. Here, we describe our recent effort toward this direction by studying the GO-induced vibrational changes of interfacial water and lipid membrane with surface-enhanced infrared absorption (SEIRA) spectroscopy. The experimental results provide evidence that overcoming the electrostatic repulsion of phosphate group, its hydrogen bonding attraction as well as the electrostatic and hydrophobic interaction of choline group are the driving forces for the effective adsorption of GO on lipid membrane. This work will open exciting new avenues to explore the use of SEIRA spectroscopy technique in probing nanobio interface.