The electrode(Ni-MWNTs) containing nickel(Ni) and multi-walled carbon nanotubes (MWNTs) was prepared by composite electrodeposit. Electrochemical hydrogen storage of the electrode was studied. The result showed a high electrochemical discharging capacity of up to 1361.1mA·h·g-1, which corresponds to a hydrogen storage capacity of 4.77Wt%(weight percent). Test of cyclic lifespan showed MWNTs had certain cyclic lifespan. Cyclic voltammetry tests showed that MWNTs can store hydrogen in chemical form.