A chromium-based low-cost metal-organic framework (MOF) cathode, MIL (Matériaux de l′Institut Lavoisier)-53(Cr), is coupled with a bioderived porous carbon (BPC) anode, produced from abundantly available agricultural waste betel nut shells in an asymmetric supercapacitor, for the first time. The impact of the electrolyte on the electrochemical behavior of an asymmetric BPC//MIL-53(Cr) supercapacitor was assessed by constructing cells with the following electrolytes: proton-conducting camphorsulfonic acid (CSA), Li+-ion-conducting solutions of LiClO4, Na+-ion-conducting sodium poly(4-styrene sulfonate) solution, and ionic liquid (IL:1-butyl-1-methyl-pyrrolidinium trifluoromethanesulfonate)-based solutions. The aqueous H+-ion-based CSA electrolyte shows a superior ionic conductivity (270 mS cm-1) and an enhanced transport number (0.96), carries larger ionic currents, and retains high conductivity even at subambient temperatures, clearly outperforming all the other Li+/Na+/IL electrolytes. The BPC/aqueous CSA or LiClO4/MIL-53(Cr) supercapacitors show enhanced storage performances, with the H+ cell having a specific capacitance of 70 F g-1 and energy and power density maxima of 9.7 Wh kg-1 and 0.25 kW kg-1 and enduring 104 cycles. A detailed account of the dependence of the electrolyte cation/anion- and solvent-type on electrochemical charge storage provides a basis for adapting these design principles to developing high-performance MOF-based supercapacitors. ©