Nowadays, unsaturated polyester resins (UPR) are mainly obtained from non-renewable resources. The ever-increasing regulations and the continuous demand for more sustainability have led to extensive research towards more environmentally suitable alternatives to petroleum-based materials. However, one of the main disadvantages of bio-based UPR is their relatively high viscosity compared to petrochemical ones. In order to overcome this drawback, in this work, we investigated the possibility to lower the resin viscosity utilizing a mixture of dimethyl itaconate (DMI) and methyl methacrylate (MMA) as a reactive diluent. The effect of the DMI and MMA ratio on resin rheological properties was investigated. The optimal curing parameters were determined and all UPRs had a high gel content, which was shown to be dependent on the DMI and MMA ratio in the formulation. Furthermore, thermomechanical and mechanical properties of the resulting network were also found to be affected by the used reactive diluent mixture. A small substitution of DMI by MMA proved to be advantageous since it offers lower resin viscosity and improved mechanical properties.

Hydrogels endure various dynamic stresses, demanding robust mechanical properties. Despite significant advancements, matching hydrogels’ strength to biological tissues and plastics is often challenging without applying potentially harmful crosslinkers. Using hydrogen bonds as sacrificial bonds offers a promising strategy to produce tough, versatile hydrogels for biomedical and industrial applications. Poly(methacrylic acid) (PMA)/gelatin hydrogels were synthesized by thermally induced free-radical polymerization and crosslinked only by physical bonds, without adding any chemical crosslinker. The addition of gelatin increased the formation of hydrophobic domains in the structure of the hydrogels, which acted as permanent crosslinking points. The increase in PMA and gelatin contents generally led to a lower equilibrium water content (WC), higher thermal stability and better mechanical properties. The values of tensile strength and toughness reached up to 1.44 ± 0.17 MPa and 4.91 ± 0.51 MJ m⁻³, respectively, while the compressive modulus and strength reached up to 0.75 ± 0.06 MPa and 24.81 ± 5.85 MPa, respectively, with the WC being higher than 50 wt.%. The obtained values for compressive mechanical properties are comparable with super-strong hydrogels reported in the literature. In addition, hydrogels exhibited excellent fatigue resistance and biocompatibility, as well as great shape memory properties, which make them prominent candidates for a wide range of biomedical applications.