Two materials currently of interest for onboard lightweight hydrogen storage applications are sodium aluminum hydride (NaAlH, a complex metal hydride, and carbon aerogels (CAs), a light porous material connected by several spherical nanoparticles. The objectives of the present work have been to investigate the synthesis, characterization, and hydrogenation behavior of Pd-, Ti- or Fe-doped CAs, NaAlH and MgHnanocomposites. The diameters of Pd nanoparticles onto CA's surface and BET surface area of CAs were 310 nm and 700900 m 2g -1, respectively. The Hstorage capacity of metal hydrides has been studied using high-pressure TGA microbalance and they were 4.0, 2.7, 2.1, and 1.2 wt for MgHFeTi-CAs, MgHFeTi, CAs-Pd, and 8 mol Ti-doped NaAlH respectively, at room temperature. Carbon aerogels with higher surface area and mesoporous structures facilitated hydrogen diffusion and adsorption, which accounted for its extraordinary hydrogen storage phenomenon. The hydrogen adsorption abilities of CAs notably increased after inclusion of metal hydrides by the hydrogen spillover mechanisms.