Redox-responsive hydrogels were prepared by mixing SS-hPG-Acry and 4-arm-PEG-SH in a 1:1 molar ratio at varying weight concentrations (%w/v) of (6%, 8%, 10%, 12.5% and 17.5%). The rheological properties of the hydrogels were compared through the elastic and viscous modulus values G´ and G´´, respectively. G' and G'' provide insights into how materials respond to deformation under oscillatory shear. G' indicates the solid-like behavior (elasticity), while G'' indicates the liquid-like behavior (viscosity). G´ and G´´ are calculated from the frequency sweep test, where the shear strain is fixed at 1% and the G´ and G´´ values are set according to the linear region when varying the frequency. The gel with lower concentrations of polymeric content exhibited lower G´ and G´´and behaved as a soft gel. At increased concentrations a noticeable increase in G´ and G´´was observed, along with increased gel stiffness (Figure ). The mesh size of the hydrogels was calculated according to the Canal-Peppas equation, with G´ as the varying parameter. Figure , showing the results of the calculations, expresses a trend of decreasing mesh size with increased polymeric content concentration; in other words, the mesh size was inversely proportional to G´. Recorded SEM images of freeze-dried hydrogels showed smaller hydrogel mesh size for hydrogels with higher concentrations of SS-hPG-Acry and 4-arm-PEG-SH (Figure ). The elastic and viscous moduli were also tested when fixing the concentration at 17.5% and varying the SS-hPG-Acry:4-arm-PEG-SH ratio. Gels did not form for a 3:1 ratio. The values of G´ and G´´increased drastically for a ratio of 1:1 and almost plateaued when further increasing the 4-arm-PEG-SH to SS-hPG ratio (Figure ). Moreover, the 17.5% gel was able to swell from its dried state, showing an almost eightfold weight increase over two hours (Figure ). The gels exhibited self-healing properties due to the dynamic nature of the disulfide bonds. To investigate these self-healing properties, extreme strain (600%) and mild strain (1%) were applied to the 17.5% hydrogel in alternating cycles (Figure ). Under 600% strain the gel was totally deformed: G´ dropped around 10 folds and became even lower than G´´. G´, as a representative of the crosslinked network density, get lower because the network collapses, losing the storage energy which is normally stored via the crosslinked network while G´´ get higher due to the applied energy that dissipates due to the lower network density which collapses when applying high shear strain force. However, when strain was reduced back to 1%, the gel showed instant recovery, with G´ and G´´returning to their original values. Thus, the hydrogels were able to conserve their viscoelastic properties and mechanical strength after their rupture if they remained partly intact. The self-healing property was also be tested visually by staining one hydrogel with a blue dye and leaving the other one uncolored. Both hydrogels were cut in half and brought in contact, then observed at different time points (Figure ). The test was performed on both 8% and 17.5% hydrogels, confirming that the gels were able to merge again, and that the 8% gel was able to heal faster.