A novel species of metal amidoborane ammoniate, [Al(NH2BH3)63−][Al(NH3)63+] has been successfully synthesized in up to 95% via the one-step reaction of AlH3·OEt2 with liquid NH3BH3·nNH3 (n = 1~6) at 0 °C. This solution based reaction method provides an alternative pathway to the traditional mechano-chemical ball milling methods, avoiding possible decomposition. MAS 27Al NMR spectroscopy confirm...