The scope of hydrogel applications can be greatly expanded by the improvement of mechanical properties. However, enhancement of nanocomposite hydrogels (NC gels) has been severely limited because the size of crosslinking nanoparticles is too large, at least in one dimension. Here we report a new strategy to synthesize non-aggregated spherulite nanoparticles, with diameters <5 nm, in aqueous solution, and their enhancement to hydrogel. The stress and stretch ratio at rupture of our NC gel are 430 and 121 KPa with only 40-p.p.m. nanoparticle content. The NC gel containing 200-p.p.m. nanoparticles can revert to 90% of its original size after enduring 100-MPa compressive stress. Our results demonstrate that the suppression of nanoparticle size without aggregation helps to establish a super stretchable and high-toughness hydrogel network at very low inorganic content.