New water-soluble nanocomposites with cobalt oxide nanoparticles (Co3O4NPs) in a poly(1-vinyl-1,2,4-triazole) (PVT) matrix have been synthesized. The PVT used as a stabilizing polymer matrix was obtained by radical polymerization of 1-vinyl-1,2,4-triazole (VT). The polymer nanocomposites with Co3O4 nanoparticles were characterized by ultraviolet–visible, Fourier-transform infrared spectroscopy, atomic absorption spectroscopy, transmission electron microscopy, dynamic light scattering, gel permeation chromatography, and simultaneous thermogravimetric analysis. The resulting polymer nanocomposites consist of spherical isolated cobalt nanoparticles with a diameter of 1 to 13 nm. The average hydrodynamic diameters of macromolecular coils are 15–112 nm. The cobalt content in nanocomposites ranges from 1.5 to 11.0 wt.%. The thermal stability of nanocomposites is up to 320 °C.