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Electrochemical double-layer capacitors (EDLCs) provide high power density and long cycle life energy storage. This work examines the use of inexpensive, raw coal char as an electrode material for supercapacitors. The effect of electrolyte composition on the performance of coal char supercapacitors is explored for the first time to determine the relative contributions of double-layer capacitance vs. faradaic reactions on total charge storage. Six electrolytes are examined with coal char electrodes, including: four aqueous electrolytes (0.5 M H 2 SO 4 , 6 M KOH, 0.5 M Na 2 SO 4 , 4 M LiNO 3 ); a water-in-salt electrolyte using 13 m NaClO 4 ; and an ionic liquid electrolyte (1-butyl-3-methylimidazolium tetrafluoroborate in acetonitrile). Voltage range, specific capacitance, electrochemical impedance, and charge–discharge characteristics of the coal char in the different electrolytes are characterized. The results indicate that neutral aqueous, water-in-salt, and ionic liquid electrolytes present a charging/discharging process approaching ideal EDLC behavior. The study provides insight into the optimal electrolyte composition for use with coal char electrodes and contributes to the current understanding of electrode-electrolyte interactions in carbon supercapacitors.