Formation of supramolecular ionic liquid (IL) gels (ionogels) induced by low-molecular-mass gelators (LMMGs) is an efficient strategy to confine ILs, and the negligible influence of LMMGs on the electrochemical properties of ILs makes ionogels ideal quasisolid electrochemical materials. Furthermore, the stimuli-responsive and self-healing characters of the supramolecular gel can be utilized for the potential development of smart electrochemical materials. However, the poor mechanical properties of supramolecular ionogels reported so far limit their practical applications. Herein, we investigated a series of efficient d-gluconic acetal-based gelators (Gn, PG16, and B8) that can harden a wide variety of ILs at low concentrations. It was shown that both alkyl chain length and the number of hydrogen bonding sites of a certain gelator, as well as the nature of the IL anion, significantly influenced the gelation abilities. The resulting ionogels were thermally reversible, and most of them were stable at room temperature. Interestingly, a PG16-based supramolecular ionogel showed rapid self-healing properties upon mechanical damage. Furthermore, the PG16-based ionogel demonstrated unprecedented performances including the favorable ionic conductivity, excellent mechanical strength, and enhanced viscoelasticity, which make it a great self-healing electrochemical material. The ionogel formation mechanism was proposed based on the analysis of Fourier transform infrared, ¹HNMR, and X-ray diffraction, indicating that a combination of hydrogen bonding, π-π stacking, and interactions between alkyl chains was responsible for the self-assembly of gelators in ILs. Overall, our present studies on exploring the structure-property relationship of gelators for the formation of practically useful supramolecular ionogels shed light for future development of more functionalized ionogels.