Polyaniline (PANI)/carbide-derived carbon (CDC) was synthesized by using in-situ chemical oxidative polymerization of PANI in presence of CDC. Conductive electrode ink materials were prepared by using eco-friendly chitosan binder in water media. In the following, symmetrical supercapacitors (SCs) were fabricated by both doctor blade coating and screen printing technique. The electrical conductivity, morphology, specific capacitance, and energy density of these composites were evaluated for their applicability as SC electrodes. Pure PANI with chitosan binder was not printable because of its brittleness, however, the presence of CDC allows the preparation of smooth films which are suitable for electrode preparation. The fabricated composite electrode has a higher specific capacitance (up to 419 F g−1) and higher energy density (up to 6.7 W h kg−1) compared to the pristine CDC electrode. The capacitance of screen-printed SCs was 440–470 mF with an equivalent series resistance of about 27 Ω.