Hydrogen fuel promises a future of renewable and clean energy. Hydrogen is the most abundant element on earth and its oxidation product water is environmentally friendly. One of the main problems with the use of hydrogen as fuel is its on-board storage. Several materials including carbon nanotubes, metalorganic frameworks, metal hydrides, graphite and activated carbon and metal/carbon nanostructures show promise as potencial materials for hydrogen storage. As an alternative to the metal hydride research, new materials based on polymers to store hydrogen are being investigated. The purpose of this work was to prepare composite materials with polyaniline and polyetherimide as matrix. The polyaniline used for this experiment was synthesized by a well-established method for the synthesis of the emeraldine base form of polyaniline using dodecylbenzenesulfonic acid as dopant. Micro particles of polyaniline/sodium alanate (NaAlH4) composite materials with 30 and 50 wt% of sodium alanate were prepared by using a spray-drying technique. In situ polyetherimide/carbon nanotubes nanocomposites with 5, 10 and 20 wt% of carbon nanotubes were also prepared. To increase the porosity of the polymer matrix, the polyetherimide was modified by sulfonation reactions, and carbon nanotubes were added during the chemical modification. The composite materials were analyzed by differential scanning calorimetry, FT-IR and scanning electron microscopy. The addition of NaAlH4 increased the stiffness of the polymer chains and increased the glass transition temperature of the polyaniline/NaAlH4 composite. The SEM images of the composites showed the formation of microspheres with NaAlH4 dispersed in the polymer matrix. Hydrogen sorption tests showed an increase in the hydrogen storage for the composites when compared to the neat materials. The values of hydrogen storage obtained in this study were higher than those found in the literature.