Protein- and polysaccharide natural-based hydrogels have been extensively used in drug delivery and tissue engineering applications due to their injectability, biocompatibility, biodegradability and processing versatility1. By means of taking advantage of the possibility of inducing the fast gelation of different polymers (e.g., gellan gum2, and alginates) in the presence of divalent ions (e.g., calcium, Ca; and manganese, Mn), we have been exploring their use in therapy and imaging, i.e. beyond the bondaries of drugs/cells delivery such as in imaging applications. In particular, Mn-based gellan hydrogel formulations have been produced and explored for Mn-MRI and treatment of ALS, under the scope of the EU-funded project NanoTech4ALS. Our most significant contributions in biomaterials and tissue engineering fields, and more recently in the development of hydrogel-based biomaterials for magnetic resonance imaging (MRI) guided delivery3 will be presented, herein. The current status quo and future trends of the hydrogels for MRI and tissue regenerationwill also be further discussed.