Among the tested carbons, only carbon aerogels (CAs) had significant effects on the hydrogen desorption behavior of LiAlH4. Adding 15 wt % CAs decreased the desorption temperature, while, with 5 wt % CAs, the desorption temperature was still the same. The desorption kinetics of the hydride with 15 wt % CAs, however, did not improve but adding 5 wt CAs resulted in desorption kinetics improvement. In addition, mixing LiAlH4 with a catalyst decreased the desorption temperature and desorption kinetics of the hydride.