A systematic investigation was conducted to synthesize hybrid composite materials that use synthetic poly-N-vinylpyrrolidone and natural (agar-agar) macromolecules with plasticizers (PEG-400) and mineral filler shungite by means of electron irradiation. The XRD and SEM data showed that the structure of the resulting hybrid composites is an interpenetrating network with distributed particles of mineral component. It has been established that the mechanical properties of hybrid composites are determined mainly by the structural organization of the interpenetrating polymer network formed under electron irradiation of the initial synthetic and natural polymer mixture in the presence of plasticizers, as well as by the conditions for intercalation of polymer segments into the mineral matrix and vice versa. It has been revealed that the degree of swelling of hybrid composites strongly depends on the concentration of a low-molecular plasticizer in the polymeric interpenetrating network, which easily impregnates into the matrix of shungite. Successfully obtained [PVP-AA-PEG] hydrogels with shungite can be applied in regenerative medicine as wound healing dressings.