This work is devoted to physical vapor deposition synthesis, and characterisation of bismuth and lutetium-substituted ferrite-garnet thin-film materials for magneto-optic (MO) applications. The properties of garnet thin films sputtered using a target of nominal composition type Bi_0.9Lu_1.85Y_0.25Fe_4.0Ga₁O₁₂ are studied. By measuring the optical transmission spectra at room temperature, the optical constants and the accurate film thicknesses can be evaluated using Swanepoel’s envelope method. The refractive index data are found to be matching very closely to these derived from Cauchy’s dispersion formula for the entire spectral range between 300-2500 nm. The optical absorption coefficient and the extinction coefficient data are studied for both the as-deposited and annealed garnet thin-film samples. A new approach is applied for accurately deriving the optical constants data simultaneously with the physical layer thickness, using a combination approach employing custom-built spectrum-fitting software in conjunction with Swanepoel’s envelope method. MO properties, such as specific Faraday rotation, MO figure of merit and MO swing factor are also investigated for several annealed garnet-phase films.