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[Display omitted] • Environmentally-friendly one-step novel method for producing rGO films. • Scale production of high-quality rGO thin films. • Applications in flexible transparent conductive films and supercapacitor electrodes. • Investigation of GO reduction mechanism, achieving valuable insights. The reduced graphene oxide (rGO) thin films have attracted much attention in flexible electronic devices and supercapacitors (SCs). However, the chemical reduction mechanism of GO needs to be clarified, and the one-step process at low temperatures for preparing high-quality rGO thin films from GO dispersions is still blank in the research field. Here, we propose a one-step operation to spray GO dispersions onto substrate or current collector under a hydroiodic acid (HI) atmosphere while simultaneously achieving the preparation of rGO thin films. This pioneering metal-free, transfer-free, fast, low-temperature, environmentally friendly, and scalable spraying technology enables large-scale production of high-quality rGO. This method realizes the preparation of highly conductive and high transmittance rGO thin films on flexible polyimide and polyethylene terephthalate substrates, as well as the preparation of rGO thin films on current collectors as SCs electrodes. Density functional theory calculations show that oxygen-containing functional groups on the surface of GO exhibit a stronger adsorption energy for HI, and have a low energy barrier during reduction by HI. Ab initio molecular dynamics simulated the possible reduction reaction path between GO and HI at 90 °C, demonstrating that HI molecules can effectively reduce GO. Furthermore, the sheet resistance of the transparent conductive film created using the method developed in this study reaches approximately 1000 Ω/sq (80 % transparency), and the specific capacitance of the SCs electrode film created in this method is 433.2 F/g (5 mV/s, 1 M H 2 SO 4). Our study not only validates the efficacy of the one-step synthesis method for rGO thin films but also provides theoretical insights into the underlying reaction mechanism. This work holds significant promise for advancing applications in various electronics by facilitating large-scale production of high-quality rGO thin films. [ABSTRACT FROM AUTHOR]