For chemical hydrogen storage, capacity is one key criterion that has spurred intense efforts to investigate compounds with high hydrogen content. The guanidinium cation and the octahydrotriborate anion possess 6 H+ and 8 H-, respectively. The combination of these two ions yields guanidinium octahydrotriborate with 13.8 wt% hydrogen. This paper presents its facile synthesis, as confirmed by 11B and 1H nuclear magnetic resonance spectroscopy. The results show that guanidinium octahydrotriborate is an ionic liquid with a melting point below -10°C, which makes it a possible injectable/pumpable hydrogen carrier. It decomposes selectively to hydrogen, in stark contrast to the formation of various boranes from related solid octahydrotriborates. The much improved H
2purity can be ascribed to the more effective combination of H+ and H-, and the higher H+/H- ratio in liquid guanidinium octahydrotriborate.