A novel Schiff base complex method was used to prepare fullerene based Ni nanocatalyst, which is used in the hydrogenation of benzene. In this method, the functionalized fullerene with primary amine was reacted with ion of nickel and salicylaldehyde. The Schiff-base complex was formed in the presence of metal ion in order to obtain the corresponding metal complex. The nickel(II) complex on C 60 shows significantly higher catalytic activity (20%) compared to the nickel bulk. Response surface methodology was also used to examine the cumulative effect of the various parameters namely, pressure, temperature, and time; thus, they were optimized to maximize the hydrogenation of benzene to cyclohexane. The optimized model predicted that the hydrogenation yield should remain maximum (very close to 100%) at reaction temperature of 150 C, reaction time of 180 min, and hydrogen pressure of 22.33 atm.