Coherent carbon cryogel-ammonia borane (C-AB) nanocomposites were synthesized, and improved H-2 storage properties are reported. Porous carbon cryogels were impregnated with AB in tetrahydrofuran solution at 25 degrees C under argon; 30% of the carbon cryogel pore volume was filled to produce a 24 wt % C-AB nanocomposite. Nitrogen sorption isotherms, X-ray diffraction, differential scanning calorimetry, differential thermal/thermal gravimetric analyses, mass spectrometry, and B-11 NMR were used to characterize the coherent C-AB nanocomposites. Findings include a merged two-step hydrogen release reaction with an appreciable reduction in the dehydrogenation temperature to < 90 degrees C as well as the suppression of borazine release. The possible nanosize effects on the H-2 storage properties are discussed.