Photocatalytic coatings with self-cleaning properties are becoming increasingly more popular due to the increased awareness of the importance of cleaning and the associated high cost of cleaning supplies and services. This research investigated self-cleaning photocatalytic polydimethylsiloxane (PDMS)/titanium dioxide (TiO2) nanocomposite coatings and focused on selecting the optimal TiO2 phase and concentration. To date, the comparison of the different TiO2 phases as a nanocomposite coating has not been sufficiently considered. PDMS/TiO2 nanocomposite coatings with three nanomaterial (NM) samples (an anatase, rutile, and mixed phase) and three concentrations of TiO2 (0.6, 1 and 3 w/v%) were prepared, applied to glass slides by dip coating, and tested with respect to hydrophobicity, surface stability, antifogging, and photocatalytic properties. It was found that a stable hydrophobic coating with the optimal photocatalyitc performance was produced with 3 w/v% anatase TiO2.