The structures of imogolite poly(acrylic acid) hydro gels were investigated using small-angle X-ray scattering (SAXS) and small-angle neutron scattering (SANS) to determine the effects of particle concentration and the magnitude of deformation. The imogolite poly(acrylic acid) hydrogel was synthesized by using gamma-ray radiation as a nanocomposite gel with chemical bonds between the particles and polymers. The SAXS measurements revealed that the imogolite network was composed of particle overlaps. Under deformation, the gel structure was rearranged to increase the dimensionality of the network, forming a relaxed structure of overlaps by changing the orientation of the imogolite. The structural response of the deformed gel depended on the imogolite concentration, which influenced the changes in dimensionality of the network and the number of overlaps. The SANS patterns indicated that the polymers wrapped the imogolite aggregates, allowing polymers to follow the imogolite behavior. These observations demonstrate that the behavior of the imogolite can contribute to both the relaxation of stress and maintenance of the structure during an applied strain.