In this study, the effects of silica-based gold-nickel(AuNi@SiO2) nanohybrid to the production of hydrogen fromdimethylamine borane (DMAB) were investigated. AuNi@SiO2nanohybrid constructs were prepared as nanocatalysts for the dimethylamine boranedehydrogenation. The prepared nanohybrid structures were exhibited high catalyticactivity and a stable form. The resulting nanohybrid,AuNi@SiO2 as a nanocatalyst, was tested in the hydrogenevolution from DMAB at room temperature. The synthesized nanohybrids werecharacterized using some analytical techniques. According to the results of thecharacterization, it was observed that the catalyst was in nanoscale and thegold-nickel alloys showed a homogenous distribution on theSiO2 surface. After characterization, the turn overfrequency (TOF) of nanohybrid prepared for the production of hydrogen fromdimethylamine was calculated (546.9 h−1). Also, theprepared nanohybrid can be used non-observed a significant decrease in activity evenafter the fifth use, in the same reaction. In addition, the activation energy(Ea) of the reaction of DMAB catalyzedAuNi@SiO2 nanohybrid was found to be 16.653 ± 1kJmol−1 that facilitated the catalytic reaction.Furthermore, DFT-B3LYP calculations were used on theAuNi@SiO2 cluster to investigate catalyst activity.Computational results based on DFT obtained in the theoretical part of the studysupport the experimental data.