Nanoporous bimetallic Fe-Ag nanoparticles (NPs) were synthesized using a facile chemical reduction method and used to decorate the surface of multi-walled carbon nanotubes (MWCNTs) for hydrogen sorption and storage. The effect of TiO2 nanoparticles on the hydrogen storage properties of Fe-Ag/CNTs was further studied in detail. For this purpose, several nanocomposites of nanoporous bimetallic Fe-Ag/TiO2 nanoparticles with different amounts of bimetallic Fe-Ag NPs were prepared via a hydrothermal method. The hydrogen storage capacity of the as-prepared nanocomposites was studied using electrochemical methods. The Fe-Ag/TiO2/CNT nanocomposite with 0.04 M bimetallic Fe-Ag NPs showed the highest capacity for hydrogen storage, which was ∼5× higher than that of pristine MWCNTs. The maximum discharge capacity was 2931 mA h g-1, corresponding to a 10.94 wt% hydrogen storage capacity. Furthermore, a 379% increase in discharge capacity was measured after 20 cycles. These results show that Fe-Ag/TiO2/CNT electrodes display superior cycling stability and high reversible capacity, which is attractive for battery applications.