Many efforts in the field of hydrogels have been focused toward increasing the mechanical strength of the gel using inorganic materials. In this study, we synthesized a hydrogel that has excellent mechanical properties using surface-modified inorganic nanofibers composed of imogolite (Al2SiO3(OH)(4)), which is a hydrated aluminum silicate that has a hollow tube structure. Gamma ray radiation generates peroxide radicals on the nanofibers (imogolite), resulting in an additive free hybrid hydrogel. Structural optimization was carried out by changing the composition of imogolite and poly(acrylic acid). Chemical bonding between the nanofiber and the polymer was simulated by a cluster model and characterized by wide area Raman spectroscopy. The results indicate that imogolite embedded in a polymer matrix can align along the direction of an elongational force, as confirmed by small angle X-ray scattering (SAXS). (C) 2013 Elsevier Inc. All rights reserved.