Ln 2 Ti 2 O 7 thin films with Ln=La to Lu were successfully grown on (110)-SrTiO 3 substrates by pulsed laser deposition. The microstructure and optical properties of the entire Ln 2 Ti 2 O 7 series were investigated by X-Ray Diffraction, Atomic Force Microscopy, Scanning Transmission Electron Microscopy coupled with Energy-Dispersive X-ray Spectroscopy and Spectroscopic Ellipsometry. For large ionic radii (i.e. Ln 3+ = La 3+ to Eu 3+), the monoclinic/layered-perovskite structure is obtained with epitaxial growth. For smaller ionic radii (i.e. Ln 3+ = Tb 3+ to Lu 3+), the cubic/pyrochlore structure is privileged. We have also observed the growth of a Gd 2 Ti 2 O 7 polymorphic phase between the stability limit of the two previously described structures. The optical band gap increases when the ionic radius of Ln 3+ decreases. Refractive index (n) and extinction coefficient (k) have been calculated over a wavelength range of 260 to 1500 nm. The low value of the extinction coefficient indicates that these materials are transparent in the visible range and can therefore be used in electrooptics systems in the case of the layered-perovskite structure and more widely as emitting materials in solid-state lasers optically pumped.