This article studies the structural and mechanical properties of polymer hydrogels based on polyelectrolyte complexes of N-succinyl-chitosan (NSC) with poly-N,N-diallyl-N,N-dimethylammonium chloride, depending on the composition of the reaction mixture and the conditions for obtaining complexes. The types of intermolecular interaction between the components of the complexes are studied by IR spectroscopy. The causes of swelling of coacervates based on polyelectrolyte complexes of N-succinylchitosan-chitosan with poly-N,N-diallyl-N,N-dimethylammonium chloride are analyzed. The relationship between the composition of coacervates and the structural-mechanical and transport properties of the gels formed from them is established. The developed approach to create elastic-viscous systems can be implemented when creating gel-like polymeric materials capable of self-organization into systems with controlled characteristics of the structure.