Herein, we report the synthesis of nitrogen-rich graphitic-carbon supported cobalt nanoparticles and their applications for the hydrogenation of various substituted nitroarenes. The aforementioned catalyst was synthesized by chelation of cobalt(II)acetate with cucurbit[6]uril unit and pyrolysis under argon atmosphere. The synthesized catalyst was characterized using various physicochemical techniques. The catalyst was very active, robust, and reusable, thus allowing selective hydrogenation of substituted nitroarenes with molecular hydrogen in a water–tetrahydrofuran solvent at 50 °C. In all cases excellent conversion and selectivity were observed with very high turnover frequency (up to 14 117 h−1).