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The research on safe and efficient hydrogen storage methods is the key scientific and technological issue which restricts the implementation of hydrogen economy. Lithium amidoborane (LiNH2BH3) has received extensive attention for its excellent hydrogen storage properties. It can desorb 10.9 wt% of hydrogen below 100 °C without deleterious by-product such as borazine. What is more, it is chemically stable at room-temperature conditions. The preparation methods and crystal structure of LiNH2BH3 were reviewed at length in this paper, and its dehydrogenation performance and mechanisms were analyzed combined with the theoretical calculation results. Moreover, the barriers and improvement measures in hydrogen release thermodynamics/kinetics and regeneration of the spent fuel were summarized. It is proposed that reducing the synthesis cost, decreasing dehydrogenation temperature with increased rates, and exploring high-efficiency, low-energy consumption, and low-cost regeneration techniques are the critical striving directions of lithium amidoborane. To the best of our knowledge, this work is the first review focusing on LiNH2BH3, one of the most promising materials for onboard hydrogen storage application, which is expected to give clues for the next advance of LiNH2BH3.