A fast proton conducting membrane has been developed by stacking graphene oxide (GO) nanosheets with some modifications, such as: compositing with cation and silk fibroin. Proton transport is promoted by such oxygen functional groups in stacked GO nanosheets, thus allowing for many potential applications, including fuel cells, water electrolysis and electrochemical gas sensor. The modified GO membrane demonstrated an expanded interlayer spacing, good stability in water, and a high proton conductivity. The device using the GO membrane sandwiched with an Ir2O3 anode and a Pt/C cathode exhibited the ability to produce hydrogen from humid air with a 100% Faradic efficiency at room temperature. In addition, flexible modified GO membrane in hydrogen gas sensing exhibited high sensitivity towards hydrogen in humid air at room temperature and up to 80oC. This study not only employs the nanocomposite material into GO layer, but also introduces a new class of flexible and robust proton conductive material based on graphene oxide membranes.