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Electrolyte-gated transistors (EGTs) represent an interesting alternative to conventional dielectric-gating to reduce the required high supply voltage for printed electronic applications. Here, a type of ink-jet printable ion-gel is introduced and optimized to fabricate a chemically crosslinked ion-gel by self-assembled gelation, without additional crosslinking processes, e.g., UV-curing. For the self-assembled gelation, poly(vinyl alcohol) and poly(ethylene-alt-maleic anhydride) are used as the polymer backbone and chemical crosslinker, respectively, and 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ([EMIM][OTf]) is utilized as an ionic species to ensure ionic conductivity. The as-synthesized ion-gel exhibits an ionic conductivity of ≈5 mS cm−1 and an effective capacitance of 5.4 µF cm−2 at 1 Hz. The ion-gel is successfully employed in EGTs with an indium oxide (In2O3) channel, which shows on/off-ratios of up to 1.3 × 106 and a subthreshold swing of 80.62 mV dec−1.