voltages for operation [1][2][3][4][5][6][7] and remarkable progress has been made in the development of semiconducting channel materials [8][9][10][11] and gate insulators. [12][13][14] The EGTs are switched on/off by applying a gate potential, which leads to a migration and local redistribution of ions at the semiconductor/electrolyte interfaces. The formed electric double layer (EDL) generates high charge accumulation in the adjacent semiconducting channel, which, for instance, renders the channel conductive at a certain gate potential. For this reason, it is important for gate insulators to show high ionic conductivities, in order to quickly develop strong EDLs that improve the EGT performance. However, the switching speed of EGTs, which is slower than that for dielectric gating, is still considered as a technical hurdle for practical applications. Therefore, various types of advanced polymer electrolytes have been intensively studied.A different approach has been established in the last few years, where an ion-gel, consisting of an ionic liquid and a poly mer, is used as a gate insulator in EGTs. [14][15][16] This approach makes use of the intrinsic properties of ionic liquids, such as high ionic conductivities, negligible volatility, and 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 selfassembled gelation, without additional crosslinking processes, e.g., UV-curing. For the self-assembled gelation, poly(vinyl alcohol) and poly(ethylene-altmaleic 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 (In 2 O 3 ) channel, which shows on/offratios of up to 1.3 × 10 6 and a subthreshold swing of 80.62 mV dec −1 .