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Electrolyte optimization plays a key role in deciding energy density (ED) and power density (PD) of supercapacitors. Increasing cell voltage is an effective way to improve ED and PD. Therefore, an electrolyte with a large potential window is highly desired. Ionic liquid (IL) electrolytes, characterized by wide potential windows, excellent thermal stability, intrinsic ionic conductivity, non-volatility, non-flammability, and low environmental concerns, are potential electrolytes and are used for micropore-and mesopore-rich activated carbon (ACmicro and ACmeso) supercapacitors. IL electrolytes consisting of various cations of EMI+ (1-ethyl-3-methyl imidazolium), PMP+ (N-propyl-N-methyl pyrrolidinium), and BMP+ (N-butyl-N-methyl pyrrolidinium) and various anions of TFSI– (bis(trifluoromethyl sulfonyl) imide), BF4 – (tetrafluoroborate), and FSI– (bis(fluorosulfonyl)imide) are explored. The electrolyte viscosity and conductivity and ion transport properties at the ACmicro and ACmeso electrodes are studied. Also, the capacitance, cycling stability, and rate capability of the ACmicro and ACmeso electrodes are systematically investigated, and post-mortem material analyses are conducted. This study shows the influence of IL composition on charge–discharge capacitances of the ACmicro electrodes is more pronounced than that for the ACmeso electrodes. The FSI-based IL electrolytes, whose electrochemical properties are dependent on cation, are found to be highly promising. Uniting EMI+ with FSI– results in low viscosity of electrolyte and high ion transport, optimizing the electrode capacitance and rate capability. Interchanging EMI+ with PMP+ enhances the cell voltage (to 3.5 V) and maximum ED (to 42 Wh kg−1) of the ACmicro cell at the cost of cycling stability.