A hydrogen storage composite and a method of forming the same are provided. The hydrogen storage composite includes a catalyst mixed with a hydrogen storage base material and a transition metal for catalyzing hydrogen desorption embedded on the surfaces of the hydrogen storage base material and the catalyst. The method includes providing at least one active metal and performing a lengthy time ball mill process to form a catalyst, providing a hydrogen storage base material to mix with the catalyst and performing a lengthy time ball mill process to form a hydrogen storage alloy material, and providing a transition metal for catalyzing hydrogen desorption to mix with the hydrogen storage alloy material and performing a shortened time ball mill process to form a hydrogen storage composite.