Two natural polymers, i.e., cellulose and water soluble pullulan, have been selectively oxidized employing the TEMPO-mediated protocol, to allow the introduction of C6-OOH groups. Thereafter, the composite hydrogels of poly(vinyl alcohol) (PVA) and different content of the oxidized polysaccharides were prepared by the freezing/thawing method. The Fourier transform infrared spectroscopy (FTIR) has been used to discuss the degree of interaction between the hydrogels constituents into the physical network. The homogeneity of the prepared hydrogels as revealed by the SEM show an excellent distribution of the oxidized polysaccharides inside the PVA matrix. The samples exhibit self-healing features, since they quickly recover the initial structure after being subjected to a large deformation. The cell viability was performed for the selected hydrogels, all of them showing promising results. The samples are able to load L-arginine both by physical phenomena, such as diffusion, and also by chemical phenomena, when imine-type bonds are likely to be formed. The synergism between the two constituents, PVA and oxidized polysaccharides, into the physical network, propose these hydrogels for many other biomedical applications.

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The excellent biological properties of chitosan (CS) together with the increased oxygen permeability of polyvinyl alcohol (PVA) were the prerequisites for the creation of a wound healing dressing that would also function as a system for L-arginine (L-arg) and caffeine (Caff) delivery. Using the freezing/thawing method, 12 hydrogels were obtained in PVA:CS polymer ratios of 90:10, 75:25, and 60:40, and all were loaded with L-arg, Caff, and the mixture of L-arg and Caff, respectively. Afterwards, an inorganic material (zeolite–Z) was added to the best polymeric ratio (75:25) and loaded with active substances. The interactions between the constituents of the hydrogels were analyzed by FTIR spectroscopy, the uniformity of the network was highlighted by the SEM technique, and the dynamic water vapor sorption capacity was evaluated. In the presence of the inorganic material, the release profile of the active substances is delayed, and in vitro permeation kinetics proves that the equilibrium state is not reached even after four hours. The synergy of the constituents in the polymer network recommends that they be used in medical applications, such as wound healing dressings.