In this study, Raney-Ni/Al2O3 catalysts were prepared from precursors which were calcined in different atmosphere (argon and air) and leached for different time. XRD, SEM, H2-TPR and BET techniques were introduced to characterize the catalysts, and hydrogenation of unsaturated hydrocarbons, including vinyltoluene, dicyclopentadiene and indene, was used as probe reaction to evaluate the catalytic hydrogenation performance of the catalysts. The results demonstrated that the calcination atmosphere had noticeable effects on the compressive strength and hydrogenation performance of Raney-Ni/Al2O3. The catalyst calcined in argon exhibited better compressive strength and catalytic performance than the one calcined in air. The compressive strength and activity stability of catalyst were also determined by the leaching time. A too longer leaching time was not conducive to improving the compressive strength and catalytic performance of catalysts. When the precursor calcined in argon was treated in a 15% (by wt.) sodium hydroxide solution at 343 K for 5 h, a catalyst with higher compressive strength (at 26.10 N/mm) was obtained and the conversion of vinyltoluene, dicyclopentadiene (DCPD), and indene could amount to more than 87.5%, 99% and even 100%, respectively, under the reaction conditions covering a temperature of 493 K, a hydrogen pressure of 2.0 MPa, a LSHV of 3.0 h?1, and a hydrogen/oil ratio of 200:1.