Among conductive polymers, poly(3,4 ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) has been widely used as an electrode material for supercapacitors, solar cells, sensors, etc. Although PEDOT:PSS-based thin films have acceptable properties such as good capacitive and electrical behaviour and biocompatibility, there are still several challenges to be overcome in their use as an electrode material for supercapacitors. For this reason, the aim of this work is to fabricate and characterise ternary nanocomposites based on PEDOT:PSS and graphene oxide (GO), blended with green additives (glucose (G) or ascorbic acid (AA)), which have the benefits of being environmentally friendly, economical, and easy to use. The GO reduction process was first accurately investigated and demonstrated by UV-Vis and XRD measurements. Three-component inks have been developed, and their morphological, rheological, and surface tension properties were evaluated, showing their printability by means of Aerosol Jet® Printing (AJ®P), an innovative direct writing technique belonging to the Additive Manufacturing (AM) for printed electronics applications. Thin films of the ternary nanocomposites were produced by drop casting and spin coating techniques, and their capacitive behaviour and chemical structures were evaluated through Cyclic Voltammetry (CV) tests and FT-IR analyses. CV tests show an increment in the specific capacitance of AAGO-PEDOT up to 31.4 F/g and excellent overtime stability compared with pristine PEDOT:PSS, suggesting that this ink can be used to fabricate supercapacitors in printed (bio)-electronics. The inks were finally printed by AJ®P as thin films (10 layers, 8 × 8 mm) and chemically analysed by FT-IR, demonstrating that all components of the formulation were successfully aerosolised and deposited on the substrate.