The fabrication of porous materials with optimized and tailored structural and chemical properties is key to their use in numerous emergent applications such as storage of electrical energy in supercapacitors, hydrogen storage, catalyst supports in fuel cells, etc. Gas and energy storage are currently attracting much attention due to the increasing demand for energy and the environmental problems caused by society’s continuing dependence on fossil fuels. Hydrogen is considered to be a clean, economical and safe renewable energy source that would be ideal to replace fossil fuels. However, it is easy to burn, which has the risk of fire and explosion. The problems of transportation and storage also restrict the application of hydrogen energy. This gas adsorbs at solid surfaces depending on the applied pressure and temperature. The development of materials for efficient hydrogen storage remains a challenge. Several studies have shown that narrow micropores are the most efficient for hydrogen storage. However, large surface area and high pore volume are also necessary to ensure high hydrogen uptake. The purpose of this work was to develop a hybrid porous materials consisting of sulfonated polyetherimide and polypyrrole blend with sodium alanate nanoparticles and carbon nanotubes. Dilute solutions with 30 wt% of hydride were first prepared under stirring at room temperature and the solutions were dried under vacuum. The hybrids were analyzed by differential scanning calorimetry, thermogravimetric analysis, transmission electron microscopy and hydrogen sorption measurements. The addition of sodium alanate changed the glass transition temperature of the hybrids when compared to the blend and the TEM images showed that simply physically mixture occurred between polymer and metallic nanoparticles. Hydrogen sorption tests showed an increase in the amount of hydrogen in the presence of higher carbon nanotubes amount.