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Screen printing has received significant attention for manufacturing energy storage devices. However, preparing high‐quality inks is still one of the main challenges. Herein, a homogenous and stable ink based on the monoclinic phase of VO2(M) microparticles has been synthesized by a simple hydrothermal process in only 6 h and through nontoxic solutions. The VO2ink is printed on Kapton substrate in a single‐layer as well as in a double‐layer arrangement (1‐LP and 2‐LP). The printed 1‐LP VO2electrode delivers a maximum areal capacitance of 20 mF cm−2with a small equivalent series resistance of 4 Ω without conducting additives. The interdigitated full‐cell VO2supercapacitor adequately employs the electric double‐layer and Faradic redox mechanisms in 1.4 V, which is the highest operating voltage reported for symmetric supercapacitors based on pure vanadium oxide electrodes in aqueous inorganic electrolytes. Moreover, the maximum areal energy of the 2‐LP supercapacitor is 0.8 μWh cm−2at an areal power of 21.0 μW cm−2, which is larger than the 1‐LP (0.2 μWh cm−2at 17.5 μW cm−2). This improvement is attributed to the homogenously printed double layer of the porous VO2microparticles. Integrating such supercapacitors into thin‐film electronics could develop portable devices. A variety of minimized electronics could be developed through cost‐effective screen printing. Preparing homogeneous and stable inks for electrochemical energy storage devices is still challenging. Pure monoclinic VO2ink has been prepared without toxic solvents and then printed in symmetric supercapacitors. In an aqueous KOH electrolyte, the operating voltage reaches 1.4 V with an areal energy of 0.8 μWh cm−2.