One of the major challenges in the field of electrochemical energy storage device performance improvement is the development of suitable synthetic materials for electrodes that can provide high power and high energy density features combined with their long-term stability. Here, we have developed a novel two-step approach based on DC glow discharge plasma pre-treatment of a carbon cloth substrate followed by electric field-assisted laser ablation for the synthesis of ZnO/C nanocomposites in a liquid and their simultaneous assembly into hierarchically organized nanostructures onto the pre-processed carbon cloth to produce a supercapacitor electrode. To form such nanostructures, a processed carbon cloth was included in the electrical circuit as a cathode during laser ablation of zinc in water, while a zinc target served as an anode. A series of studies have been performed to explore the structure, morphology, composition and electrochemical characteristics of the synthesized ZnO/C nanocomposites. Application of the external field provided additional possibilities for tuning the particle morphology. The parameters of the obtained nanostructures were shown to depend on the direction of the applied electric field and liquid composition. SEM studies revealed a nanoflower-like morphology of the prepared nanomaterial having potential in supercapacitor applications due to a large surface area. The ZnO/C nanoflowers, deposited onto a carbon cloth substrate, were tested for energy storage by cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) analysis. The results showed a pseudocapacitor behavior with a maximum specific capacitance of about 3045 F g-1 (at a scan rate of 1 mV s-1). These results demonstrate a promising storage efficiency of the synthesized ZnO/C nanocomposite as a material for supercapacitors.