The study comprehensively investigates the design and performance of self-cleaning surfaces fabricated by coating aluminum foil with an acrylic paint matrix enriched with different content of titanium dioxide (TiO2) nanoparticles. The main goal was to assess the self-cleaning characteristics of the surfaces obtained. This study employs scanning electron microscopy (SEM) to analyze the morphology of TiO2-modified acrylic surfaces, revealing spherical particles. Raman spectroscopy elucidates signatures characterizing TiO2 incorporation within the acrylic matrix, providing comprehensive insights into structural and compositional changes for advanced surface engineering. Alternating current (AC) impedance spectroscopy was used to assess selected charge transport properties of produced self-cleaning surfaces, allowing us to gain valuable insights into the material’s conductivity and its potential impact on photocatalytic performance. The self-cleaning properties of these tiles were tested against three frequently used textile dyes, which are considered to pose a serious environmental threat. Subsequently, improving self-cleaning properties was achieved by plasma treatment, utilizing a continuous plasma arc. The plasma treatment led to enhanced charge separation and surface reactivity, crucial factors in the self-cleaning mechanism. To deepen our comprehension of the reactive properties of dye molecules and their degradation dynamics, we employed a combination of density functional tight binding (DFTB) and density functional theory (DFT) calculations. This investigation lays the foundation for advancing self-cleaning materials with extensive applications, from architectural coatings to environmental remediation technologies.