A pore-lining coating method for marble stone surfaces based on the fluorosurfactant Capstone FS-63 has been optimized for application through spray coating by tuning the solvent composition. The optimized application conditions showed an effective penetration depth of the hydrophobic properties down to at least 0.5 mm, ensuring a long-term protection against water uptake. Mechanistic studies of the functionalization process revealed that the solution mixtures containing ethylene glycol provide the best pore-lining functionalization, due to the prolonged functionalization time as a consequence of the slow evaporation rate of the solvent combined with the beneficial shift in the surfactant-vesicle equilibrium towards free surfactants. The coatings also display anti-graffiti properties, allowing for graffiti paint to easily be washed away with a standard pressure washer repeatedly 3–4 times. For optimal re-usability of the anti-graffiti coatings, a new coating can be applied when the first coating loses its effectiveness.