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The reduction of nitroaromatics is important in industrial wastewater treatment. However, the activity of an external catalyst is critical for the reaction. In this study, Au nanocrystals were anchored in situ on two-dimensional graphene oxide (GO), which had oxygen-rich groups on its surface. Oxygen-containing groups combined to form functional boron clusters through hydrogen bond interactions (BGO). The mild reducibility of a dodecahydrododecaborate anion cluster (closo-[B12H12]2−) made ultrafine Au nanocrystals uniformly disperse on GO (Au/BGO). 4-Nitrophenol and other nitro-aromatic hydrocarbons could be rapidly hydrogenated into aminoaromatic hydrocarbons by Au/BGO, and the hydrogenation efficiency was approximately 100%. It retained high catalytic activity after 16 catalytic cycles. Therefore, the proposed innovative preparation strategy and high catalytic activity indicate the advancement of closo-[B12H12]2− as a nucleation target for nanometals. This study provides a stable and efficient catalyst for the hydrogenation of nitroaromatics and an alternative approach for the preparation of supported nano-metals.