It is of great interest to develop and utilize a high surface area material with optimized hydrogen sorption properties. The need for a renewable energy source to replace automobile gasoline has become more critical in the past decade. Hydrogen is a viable fuel source for automobile usage; however, the question of how hydrogen will be safely and efficiently stored still remains. Critical factors for optimum hydrogen storage include ambient conditions and low activation temperature for adsorption and desorption phenomena. In order for optimum hydrogen adsorption to be achieved, the properties of (1) high surface area, (2) optimum hydrogen adsorption energy, and (3) Kubas interactions between metals and hydrogen molecules need to be considered. Fullerenes have recently become more popular with the discovery and mass production of graphene sheets derived from graphite. Graphene is a modified form of graphite that takes the form of sheets with less agglomeration than its respective graphitic form. This form has the potential for high surface area and storage capabilities. Storage of hydrogen at room temperature must be optimized by increasing the surface area and having an adsorption enthalpy between 15 - 20 KJ/mol. Graphene (G) sheets and graphene oxide (GO) sheets have been utilized as a matrix for hydrogen storage. These materials can also be cross-linked with organic spacers in order to form a porous framework of higher surface area. Metal decorating by calcium and platinum of the G/GO matrix has been used to enhance Kubas interactions, adsorption enthalpies, and spillover phenomenon. The use of a polymer matrix has also been implemented. Polyaniline is a novel superconducting polymer with unique electronic properties. Complexes of Polyaniline with graphene and graphene oxide have been investigated for hydrogen storage properties. Graphene and graphene oxide surface modification via metal decoration have been investigated in order to determine the most efficient synthesis and particle size on the G/GO matrix. Characterization by XRD, BET, adsorption enthalpy, PCT, TGA, FT-IR, and TEM/SEM (when applicable) were employed to optimize and compare the materials in the effort to develop a suitable storage material.