A study of synthesis of multi-walled carbon nanotubes (MWNTs) and carbon sphere and also their electrochemical performance for the storage hydrogen gas has been presented. The structure and the morphology of carbon nanostructures have been investigated using X-ray diffraction, scanning electron microscopy, transmission electron microscopy. Furthermore, the electrochemical hydrogen adsorption properties of MWNTs and carbon spheres were elucidated by galvanostatic charge/discharge and cyclic voltammetric measurements. The electrochemical results demonstrated that carbon spheres synthesized from sucrose and starch exhibited hydrogen adsorption of ∼0.9 and 1 wt% respectively. Whereas, the multiwalled carbon nanotubes have exhibited hydrogen adsorption of ∼1.2 wt%.