This study investigates the characterization and performance of self-cleaning TiO2 surfaces synthesized through a one-step preparation process, followed by enhancement via plasma treatment. The process involved coating aluminum foil with an acrylic paint mixture containing nanoparticles of different mass compositions and subsequent plasma treatment using a continuous plasma arc. Scanning electron microscopy revealed the morphology of the treated surfaces, showing an increase in surface area of plasma-treated materials. Energy-dispersive X-ray spectroscopy revealed changes in oxygen and titanium in acrylic paint/TiO2 surfaces as the TiO2 content increased, indicating successful TiO2 incorporation. Raman spectroscopy showed that the bulk structure of self-cleaning acrylic paints is mainly preserved after plasma treatment. Alternating current impedance spectroscopy assessed that plasma treatment reduced agglomeration and increased active sites, especially for the acrylic paint/TiO2 surfaces with 0.5 mg/cm3 TiO2. The contact angle measurements indicated that plasma treatment enhanced the superhydrophobic characteristics and potential self-cleaning abilities of produced acrylic paint/TiO2 surfaces. The efficacy of these plasma-treated surfaces in self-cleaning was evaluated by testing their performance against puddle sediment and automotive oil samples. The study demonstrated that plasma treatment positively impacted the self-cleaning ability of the acrylic paint/TiO2 surfaces, particularly those with 0.5 mg/cm3 TiO2. This enhancement was attributed to the formation of functional groups, improved water repellency, and possible increases in surface area, which collectively contribute to the sustainable self-cleaning properties of the treated surfaces.