Amyloid β (A β) is a potential biomarker of Alzheimer's disease (AD), and its fibrillation behavior is of interest and value. In this study, the A β behaviors on phospholipid membranes were observed by Membrane Surface-Enhanced Raman Spectroscopy (MSERS) method. Phospholipid (PL) membranes, consisting of DMPC and DMPS with a molar ratio of 9:1, were fabricated on gold nanoparticles with diameter of 100 nm (Au@PL). Enhancement of the Raman intensity of Au@PL was increased by A β, with enhancement factor about 40. The H-bonding network was disturbed in presence of NaCl which covered Au@PL and made Au@PL away from one another. When A β was applied with Au@PL, the H-bonding network was disturbed just after mixing. As the reaction reaches to equilibrium, A β attracted neighbouring Au@PL and induced aggregation of Au@PL which blocked the aggregation prone site of A β to inhibit further fibrillation. Based on our method, the A β behaviors at lipid membrane surface can be directly observed via enhanced Raman signals.