The accumulation of crystallization deposits at the surface of heat exchangers results in the increase of the heat transfer resistance and a drastic loss of efficiency. Coating surfaces with a thin film can limit the scale-surface adhesion force and thus the fouling process. This study compares the efficiency of TiO2 layers exhibiting various crystalline planes and microstructures to reduce the kinetic of fouling. Molecular modelling with density functional theory is first carried out to determine the energy of CaCO3 deposition on anatase (101), (004), and (200) surfaces as well as on a rutile (101) one. TiO2 thin films (thickness < 1 μm) are then synthesized by direct current and high power impulse magnetron sputtering (dcMS and HiPIMS respectively) in order to tune their crystallinity and microstructure. Lastly, the induction time to grow CaCO3 crystals at the surface of such materials is determined. Comparing the modelling and fouling results allows to draw general trends on the potential anti-scaling properties of TiO2 crystallized under various forms. Until now, such a comparison combining a theoretical approach with experimental fouling tests has never been reported in the literature.