We have produced complex lithium-containing nitrides as nanostructures in which it is possible to control the morphology through carefully tailoring the synthetic conditions. We observe that the nanomaterials store hydrogen with a significant improvement in sorption kinetics and cyclability compared with the bulk materials. Notably, bulk lithium nitride synthesised using liquid metal methods exhibits a total hydrogen storage capacity greater than 10 wt. % at 200°C and will store ca. 4 wt. % hydrogen reversibly. Storage capacity in the bulk material was observed to improve on successive cycles between the imide and amide phases. At the same temperature of 200°C nanostructured lithium nitride exhibits a total hydrogen storage capacity of ca. 9 wt. % and stores in excess of 5 wt. % hydrogen reversibly. It is also noteworthy that our nanostructured nitride reaches its optimum gravimetric capacity with an approximate three-fold increase in rate compared with the bulk material.