Separation of itaconic acid from aqueous solution has been explored using various carbon-based adsorbents obtained from the pyrolysis and KOH activation of coconut shell biomass. The best preparation conditions to obtain a tailored adsorbent for itaconic acid purification were identified via a Taguchi experimental design, where its adsorption properties were maximized. The best activated carbon was obtained via coconut shell pyrolysis at 750 °C for 4 h plus an activation with 0.1 KOH and a final treatment at 800 °C for 2 h. This adsorbent showed an adsorption capacity of 4.31 mmol/g at 20 °C and pH 3 with a surface area of 466 m2/g. Itaconic acid separation was exothermic and pH-dependent where electrostatic forces and hydrogen bonding were the main adsorption interactions. Calculated adsorption rate constants for itaconic acid adsorption were 0.44–1.20 h-1. Results of adsorbent characterization analysis indicated the presence of a crystallization of itaconic acid molecules onto the activated carbon surface where 3–4 molecules could interact to form the clusters. This organic acid was recovered from the adsorbent surface via desorption with water or ethanol, thus facilitating its final purification. The best activated carbon obtained in this study is a promising alternative to perform sustainable and energy-efficient downstream separation and purification of itaconic acid produced via fermentation.