Novel composite hydrogels based on poly(acrylic acid-co-acrylamide)/polyacrylamide pseudo-interpenetrating polymer networks (pIPNs) and magnetite were prepared via in situ precipitation of Fe3+/Fe2+ions within the hydrogel structure. The magnetite formation was confirmed by X-ray diffraction, and the size of the magnetite crystallites was shown to depend on the hydrogel composition: the crystallinity of the magnetite particles increased in line with PAAM content within the composition of the pIPNs. The Fourier transform infrared spectroscopy revealed an interaction between the hydrogel matrix, via the carboxylic groups of polyacrylic acid, and Fe ions, which strongly influenced the formation of the magnetite articles. The composites’ thermal properties, examined using differential scanning calorimetry (DSC), show an increase in the glass transition temperature of the obtained composites, which depends on the PAA/PAAM copolymer ratio in the pIPNs’ composition. Moreover, the composite hydrogels exhibit pH and ionic strength responsiveness as well as superparamagnetic properties. The study revealed the potential of pIPNs as matrices for controlled inorganic particle deposition as a viable method for the production of polymer nanocomposites.