Industrial catalyst waste has emerged as a hazardous pollutant that requires safe and proper disposal after the unloading process. Finding a valuable and sustainable strategy for its treatment is a significant challenge compared to traditional methods. In this study, we present a facile method for the recovery of molybdenum and aluminum contents from spent Mo-Ni/Al2O3 hydrogenation catalyst through crystallization separation and coprecipitation. Furthermore, the recovered molybdenum and aluminum are utilized as active metals and carriers for the preparation of new catalysts. Their properties were thoroughly analyzed and investigated using various characterization techniques. The hydrogenation activity of these newly prepared catalysts was evaluated on a fixed-bed small-scale device and compared with a reference catalyst synthesized from commercial raw reagents. Finally, the hydrogenation activity of the catalysts was further assessed by using the entire distillate oil of coal liquefaction as the raw oil, specifically focusing on denitrogenation and aromatics saturation. This work not only offers an effective solution for recycling catalyst but also promotes sustainable development.