Excimer laser (lambda = 308 nm, tau = 10 ns) and electron beam (W = 7 MeV) irradiation effects in Fe-57:LiNbO3 have been studied on samples of two crystallographic orientations. Complementary information regarding radiation induced changes to the optical absorbance of the crystal, valence states of Fe, phase composition and morphology of the irradiated regions was obtained by optical absorption measurements, Mossbauer spectroscopy, scanning electron microscopy (SEM), energy dispersive X-ray (EDX) spectroscopy, microRaman and Read thin film camera analysis. The relationship between irradiation treatment conditions and induced property modifications in iron-doped lithium niobate is reported within the frame of available defect models.