Storing hydrogen efficiently in condensed material under mild conditions is a key technique challenge. Here, we developed a new family of hydrogen storage material spanning across the domain of inorganic and organic hydrides, namely metalorganic hydrides, utilizing the electron donating nature of alkali or alkline earth metals to tune the thermodynamic property of hydrogen storage. Theoretical calculations reveal that the extent of δHd reduction of the metalorganic hydrides is dependent on the electronegativity of metal. In line with our calculation results, a series of metalorganic hydrides were successfully synthesized, among which two new structures were solved. Furthermore, their hydrogen absorption and desorption reversibility were successfully exemplified with lithium carbazolide, which has a hydrogen capacity of 6.5 wt% and δHd of 33.7 kJ mol-1-H2 that is superior to its parent substance.