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We report for the first time the reversible hydrogen storage behavior at room temperature in polyaniline nanofibers. The rate of hydrogen sorption during the initial run was very rapid and an extended plateau pressure of about 30 bars was obtained from the pressure-composition isotherm profiles of these polyaniline nanofibers. The reversible cycling capacity of approximately 3-4 wt% was demonstrated at room temperature and has been attributed to the unique nanofibrous microstructural and surface properties.