The rational modulation of catalysts with efficient hydrogen activation and controllable management properties is essential to improve the hydrogenation performance. Herein, we have employed a gradient diffusion-in situ reconstruction strategy to prepare the YS-Co3S4@AlO-CoMoS catalyst with an efficient hydrogen spillover network. The coordinated dissociation of Co-hybrid nanospheres during sulfidation promotes gradient diffusion of Co2+ and drives its binding with small-sized (NH4)3[AlMo6O24·6H