Green low-cost synthesis and efficient recyclability are two major hindrances for Au nanocrystals as catalysts applying in diverse industrial reaction processes. By the use of low-cost α-zein (i.e. a major storage protein of corn) as the reductant, capping agent and stabilizer, Au nanocrystals with tunable catalytic activity were synthesized in a wet-chemical approach. Fibrillation of α-zein further enhanced its reducing ability due to larger specific surface area and more hydrophilic groups exposed on the surfaces. The obtained Au nanocrystals had biocompatibility, high stability in various solvents, unique solubility in aqueous alcohol and high catalytic ability, being able to detect ethanol composition in aqueous ethanol as well as H2O2 for diagnosis of diabetes mellitus. These advantages also enable efficient recyclability of Au nanocrystals with continuous flow catalysis in different solvents and environments. Thus, the use of α-zein offered Au nanocrystals not only with green low-cost synthesis, but also with tunable catalytic activities, ethanol-responsiveness and efficient recyclability, which may be applicable in diverse fields.