The incessant developments in the pharmaceutical and biomedical fields, particularly, customised solutions for specific diseases with targeted therapeutic treatments, require the design of multicomponent materials with multifunctional capabilities. Biodegradable polymers offer a variety of tailored physicochemical properties minimising health adverse side effects at a low price and weight, which are ideal to design matrices for hybrid materials. PLAs emerge as an ideal candidate to develop novel materials as are endowed withcombined ambivalent performance parameters. The state-of-the-art of use of PLA-based materials aimed at pharmaceutical and biomedical applications is reviewed, with an emphasis on the correlation between the synthesis and the processing conditions that define the nanostructure generated, with the final performance studies typically conducted with either therapeutic agents by in vitro and/or in vivo experiments or biomedical devices.

Creating flexible, high-strength hydrogels from harmless, low-cost natural polymers is an area of intense research today due to their potential applications in the biomedical field, which demands materials with ambivalent physicochemical features. In particular, great efforts were devoted to the preparation of sustainable biohydrogels, composed of hydrophilic networks of renewable, biocompatible, biodegradable and low-cost biopolymers. Bionanocomposites are a promising synthetic approach to combine specific multifunctional materials with targeted physicochemical properties. Novel bionanocomposite hydrogels were designed by combining both chondroitin sulfate (CS) as well as gelatin (GE) obtained from the waste generated by the fish industries to form double fibre networks with tailored properties. In addition, hybrid bionanocomposites were achieved by introducing graphene nanoparticles (xGnP) into the double fibrillar network (GE/CS) to enhance the physicochemical properties. The bionanocomposite nanostructures were characterized by Fourier transform infrared spectroscopy (FTIR), differential scanning calorimeter (DSC) whilst their rheological properties and thermal stability were determined by rheological and thermogravimetric analyses (TGA), respectively.The likely interactions between CS and gelatin in the GE/CS hydrogel network were proved by ATR-FTIR spectroscopy. The incorporation of xGnP improved the mechanical properties of the GE/CS fibrillary network by an order of magnitude in the shear storage modulus.Eventually, the generated bionanocomposites hydrogels and bionanocomposite hybrid hydrogels have promising potential for applications in many biomedical fields, including drug delivery and tissue engineering by mimicking tissue extracellular matrix components such as the gelatin for collagen and the CS in the cartilage.