This invention discloses a high-hydrogen-density liquid organic hydrogen carrier and its applications, belonging to the field of hydrogenenergy storage and utilization technology. The liquid organic hydrogen carrier is a composite system of a functionalized nitrogen-containing heterocyclic compound and a metal-organic framework material supported on a non-precious metal catalyst. The nitrogen-containing heterocyclic framework is connected with electron-donating and electron-withdrawing groups, constructing an intramolecular electron push-pull system. The non-precious metal catalyst is supported inside the pores or on the surface of the metal-organic framework material. Through molecular structure design and catalyst system optimization, this invention achieves a hydrogen storage density of not less than 7.0 wt%, a dehydrogenation onset temperature of not more than 150℃, and a dehydrogenated hydrogen purity of not less than 99.99%, with excellent cycle stability and low catalyst cost. This liquid organic hydrogen carrier can be widely used in renewable energy storage, long-distance hydrogen transportation, vehicle-mounted hydrogen sources, and distributed energy supply systems.