Polymer nanocomposite gels (NC gels), a kind of typical soft materials, can be synthesized through free-radical polymerization of water-soluble monomers in the presence of nanoclay in aqueous system. Here, novel natural tube-like nanoparticles, halloysite nanotubes (HNTs), are firstly used as multifunctional cross-linkers for polyacrylamide (PAAm) to form a new type of organic/inorganic hybrid hydrogels. Significant improvements in mechanical properties of the PAAm-HNTs NC gels are found by the addition of HNTs as shown by the static mechanical testing and dynamic viscoelasticity measurement. HNTs are uniformly dispersed in the NC gels from the morphological result. HNTs can be intercalated by PAAm chains as observed by the X-ray diffraction result. Hydrogen bonding interactions between HNTs and PAAm are confirmed by the infrared spectroscopy and X-ray photoelectron spectroscopy. The maximum equilibrium degree of swelling (EDS) for the NC gel is 4000% and the EDS decreases with the concentration of clay nanotubes. The present work provides a novel routine for preparing NC gels using “green” one-dimensional nanoparticle. The prepared NC gels have promising application in biomedical areas due to the superior mechanical properties of the gels and good biocompatibility of HNTs.