Recently, supramolecular hydrogels have attracted increasing interest owing to their tunable stability and inherent biocompatibility. However, only few studies have been reported in the literature on self-healing supramolecular nucleoside hydrogels, compared to self-healing polymer hydrogels. In this work, we successfully developed a self-healing supramolecular nucleoside hydrogel obtained by simply mixing equimolar amounts of guanosine (G) and isoguanosine (isoG) in the presence of K+ . The gelation properties have been studied systematically by comparing different alkali metal ions as well as mixtures with different ratios of G and isoG. To this end, rheological and phase diagram experiments demonstrated that the co-gel not only possessed good self-healing properties and short recovery time (only 20 seconds) but also could be formed at very low concentrations of K+ . Furthermore, nuclear magnetic resonance (NMR), powder X-ray diffraction (PXRD), and circular dichroism (CD) spectroscopy suggested that possible G2 isoG2 -quartet structures occurred in this self-healing supramolecular nucleoside hydrogel. This co-gel, to some extent, addressed the problem of isoguanosine gels for the applications in vivo, which showed the potential to be a new type of drug delivery system for biomedical applications in the future.