The classical organic semiconducting material used for OECTs is an ionomer mixture called poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), comprising of a conjugated PEDOT phase and a deprotonated PSS phase. Holes in the PEDOT phase is compensated by the negatively charged sulfonate ions in the PSS phase, making the PEDOT phase conducting. In the absence of a gate bias (V GS = 0 V), the flow of mobile holes within the polymer maintains a hole current when a drain voltage (V DS) is applied (ON state). By applying a positive gate voltage (V GS > 0 V), cations from the electrolyte are injected into the channel and PSS anions are charge compensated, initiating the dedoping of PEDOT, reducing the hole density and thus lowering the drain current (OFF state). Such mode of operation is known as depletion mode; the OECT is ON in the absence of a gate bias. It is also possible to operate the OECT in accumulation mode if the conjugated polymer does not consist of any native dopants. Accumulatedmode OECT is typically in the OFF state and application of a negative gate voltage leads to injection of anions into the semiconducting polymer, initiating an electrochemically driven hole accumulation in the channel, leading to the ON state. Recently, naphthalene diimides (NDIs)-based polymers, [15] ladder-type polymers such as poly(benzimidazobenzophenanthro-line) (BBL), [16] fullerene derivatives with glycolated side chains, [17] and random copolymer with glycol side chain such as P-90 [9,18] were reported to be promising n-type materials to develop accumulation mode OECTs with stable operation in aqueous environments. Another class of promising p-type materials for accumulation mode OECTs is semiconducting polymers based on benzodithiophene or bithiophene core with glycol side chains, [19,20] glycolated thiophene (g2T-T) polymers, [21] poly(3hexylthiophene) (P3HT), [22,23] conjugated polyelectrolytes based on poly(6-(thiophene-3-yl)hexane-1-sulfonate) tetrabutylammonium (PTHS), [24] polythiophene derivative with ethylene glycolbased side chains (P3MEEMT), [12] and poly(6-(thiophen-3-yl) hexane-1-sulfonate) tetrabutylammonium (PTHS:TEA). [25] Generally, the material must have simultaneously an aggregated, interconnected structure that supports efficient hole transport, and an amorphous phase to hydrate, and thus enable the transport of ions. The in-depth introduction on active materials for OECTs can be found in several review papers. [26-30] The key feature of OECT is that the transition of doping/ dedoping states occurs over the entire channel volume, as Organic electrochemical transistors (OECTs), where conjugated polymers undergo doping/dedoping from an electrolyte, are widely studied for applications ranging from switching elements, artificial synapses to transducers for biological sensing. The concurrent transport of electronic and ionic charges within the channel provide OECTs with excellent amplification capability and efficient ion-to-electron transduction at low operating voltages (<1 V). Herein, the la...