The synthesis and study of metal-containing hydrogels, particularly those filled with nickel nanoparticles, is currently of interest to many researchers. This paper presents the results of an investigation of the structure and properties of Ni(0)-filled composites on the basis of 2-hydroxyethylmethacrylate copolymers (HEMA) with polyvinylpyrrolidone (PVP) and their hydrogels. The authors of the article are the first who propose the method to produce these materials by combining the processes of polymer matrix synthesis and a reduction of Ni2+ ions. Synthesis is carried out in one stage without complicated equipment and is technologically simple. It is determined by thermometric research that the temperature conditions required for the chemical reduction of Ni2+ are achieved due to the heat released during the exothermic reaction of HEMA polymerization in the presence of PVP. With the help of Fourier transform infrared analysis, and thermogravimetric and differential-thermal analysis, the formation of a crosslinked graft copolymer based on HEMA and PVP was confirmed, and its structural parameters, including the efficiency of PVP grafting, PVP content in the copolymer, and the molecular weight of the interstitial fragment of the polymer network, were investigated. The results obtained with scanning electron microscopy revealed that the size of the Ni(0) particles is about 500 nm. X-ray structural analysis of the composites obtained confirmed the existence of metal nickel particles. The strength, elastic, sorption, electrical, and magnetic properties of the obtained composites in the solid (dry) and elastic (swollen) physical states, depending on the composition of the copolymer and the content of the metal filler, have been investigated.