Palladium nanoparticles were successfully prepared on a nanodiamond (ND) support and used for the hydrogenating deamination of benzonitrile, aromatic imines, and amines for the first time. The developed methodology was further used for the in situ conversion of aldehydes into hydrocarbons, including a biomass‐derived model compound. The activity of the catalyst was compared with palladium supported on activated carbon (AC) under identical conditions and the performance of Pd/ND was found to be superior to Pd/AC. The origin of the difference in the catalytic performance was considered. Finally, an attempt has been made to understand the mechanism through the identification of the side products by GCMS analysis.