The polyelectrolyte complexes formed due to electrostatic attraction between the polymers, have improved properties when compared to hybrid CTS-g-GMA, which provides a wide range of applications in the biomedical field. All materials have been characterised by different analytical techniques such as infrared spectroscopy (FTIR), X-ray diffraction (XRD), thermal analysis (DSC and TGA), and the results were compared to the precursor materials (chitosan, X, HA, and CTS-g-GMA). Due to the HA nature, the film obtained from this reaction has been assessed for use as a patch for wound healing; whereas the properties showed by the hydrogels obtained from the reaction with X, make them very promising for applications in the treatment of recovery of spinal cord injuries. This book presents results which strongly support the future use of hydrogels as scaffolds for tissue engineering and recovering.