Lack of efficient hydrogen storage method is one of the technical bottlenecks for the implementation of hydrogen energy. Liquid organic hydrogen carriers (LOHCs), especially Nheterocycles, have been considered as potential candidates for both on-board and off-board hydrogen storage owing to their low cost, high gravimetric hydrogen storage capacity, reversibility, and compatibility with the existing infrastructures with minimal modification. LOHCs however encounter severe kinetic barriers in the hydrogen uptake and release processes, and thus efficient catalysts are critically needed. Much attention has been given to the design and development of catalysts for the reversible hydrogenation and dehydrogenation of N-heterocycles. In this Mini-Review Article, we summarize recent activities in advancing those compounds for hydrogen storage through thermo-, photo-, and electrocatalysis, aiming to provide a guidance for rational catalyst design. At the end of the Mini-Review Article, challenges and future research directions of the catalyst design in the LOHCs field are discussed.