The lack of cost-effective regeneration techniques for LiBH4 limits its large-scale applications for supplying hydrogen via hydrolysis. Now, we report a facile method to regenerate LiBH4 by ball milling its real hydrolytic byproduct (LiBO2·xH2O) with cheap Al based reducing agents, instead of traditional Mg. Effective strategies are developed to promote the formation of LiBH4 by introducing Li2O to enable the dense Al2O3 to convert into LiAlO2 on Al surface and break up passivation layers, and by partially replacing Al with Al-RE alloy to improve grinding and contacting efficiency of raw materials and facilitate the conversion from initial H+ in LiBO2·2H2O to final H¯ in LiBH4. A yield of 10.4 % can be obtained for a relatively short ball milling time (10 h) for the Al-Al2Ce-Li2O-LiBO2·2H2O system. Another advantage of this method is that the utilization of H+ source in LiBO2·2H2O improves energy efficiency and reduces the cost. This work broadens the species of reducing agents for borohydride regeneration and enriches its regeneration methods.