“…Supramolecular noncovalent forces, including hydrogen bonding, electrostatic interactions, donor–acceptor associations, hydrophobic effects, and π–π stacking, are essential in forming supramolecular gel materials directed by low-molecular weight gelators. − Supramolecular gels have gained prominence as versatile materials with a wide range of applications, including their use in chemosensors, lithography, electrochemical devices, catalysis, adsorption and removal of toxic dyes, optoelectronic devices featuring conjugated oligomers, polythiophenes, phthalocyanines, and tetrathiafulvalenes, drug delivery systems, cellular supports, tissue engineering, and antimicrobial and anticancer activities. − The incorporation of various transition and inner transition metal ions into the supramolecular gel network introduces a range of additional beneficial characteristics, including magnetic activity, optical activity, and semiconducting properties. − The current decade places significant emphasis on the design and synthesis of self-repairing metallogels, owing to their extended lifespan and multifaceted applications. − Recent research findings underscore the significance of factors such as the polarity of various chemical components, extensive π-electron delocalization, and intra- and intermolecular hydrogen bonding interactions, as pivotal contributors to the formation of self-healing metallogels and the emergence of their nonlinear optical properties. − It is legitimate to propose that self-healing behavior and optical nonlinearity are closely intertwined phenomena. In earlier research, we had explored the development of transparent metallogels using Cu(II) metal salts and macromolecular gelators like BSA protein and investigated their nonlinear optical properties .…”