Abstract <p>The current upsurge in the electronics industry has paved the way for increased demand for high-performance conductive nanocomposites for various applications, including energy storage, sensors, electronic devices, and aerospace. Despite their extensive applications, several challenges have remained, specifically concerning these composites' complex synthesis and time-consuming production process. In this research, low-temperature aerosol-assisted atmospheric pressure plasma was innovatively exploited for directly depositing rGO-PANI nanocomposite thin films in two configurations (single-step and layer-by-layer) on dielectric substrates under atmospheric conditions. Subsequently, the chemical properties and morphological characteristics of the rGO-PANI nanocomposite thin films, deposited via aerosol-assisted plasma, were investigated. As a proof of concept, the use of rGO-PANI nanocomposite films of various structures was investigated as a selective ammonia gas sensor by measuring the variations in their electrical resistance within the concentration range of 100–400 ppm at constant experimental conditions (room temperature: 25 ± 1&#xa0;°C, relative humidity: 40 ± 5%). The results revealed the fast response, high stability, and distinct selectivity of the chemiresistive gas sensor at room temperature. The developed aerosol-assisted plasma deposition technology can be considered a new step in the low-cost, rapid, and feasible production of efficient conductive nanocomposite films for electronic applications.</p> Graphical Abstract <p></p>