Environmentally friendly energy storage devices have been fabricated by using functional materials obtained from completely renewable resources. Gelatin, chitosan, casein, guar gum and carboxymethyl cellulose have been investigated as sustainable and low-cost binders within the electrode active material of water-processable symmetric carbon-based supercapacitors. Such binders are selected from natural-derived materials and industrial by-products to obtain economic and environmental benefits. The electrochemical properties of the devices based on the different binders are compared by using cyclic voltammetry, galvanostatic charge/discharge curves and impedance spectroscopy. The fabricated supercapacitors exhibit series resistance lower than a few ohms and values of the specific capacitance ranged between 30 F/g and 80 F/g. The most performant device can deliver ca. 3.6 Wh/kg of energy at a high power density of 3925 W/kg. Gelatin, casein and carboxymethyl cellulose-based devices have shown device stability up to 1000 cycles. Detailed analysis on the charge storage mechanisms (e.g., involving faradaic and non-faradaic processes) at the electrode/electrolyte interface reveals a pseudocapacitance behavior within the supercapacitors. A clear correlation between the electrochemical performances (e.g., cycle stability, capacitance retention, series resistance value, coulombic efficiency) ageing phenomena and charge storage mechanisms within the porous carbon-based electrode have been discussed. © 2021 by the authors. Licensee MDPI, Basel, Switzerland.

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