Since 2007, at the Electron Science Research Institute (ESRI) nano-fabrication laboratories, Edith Cowan University, Australia, we have devoted research efforts to the synthesis and characterization of bismuth-containing ferrite-garnet-type thin-film magneto-optic (MO) materials of different compositions. We report on the development and properties of highly bismuth-substituted iron-garnet thin films prepared by using radio frequency (RF) magnetron sputtering. We study the process parameters associated with the RF magnetron sputter deposition technique and investigate the results of optimizing process parameters and implementing several special techniques including the fabrication of co-sputtered nanocomposite films, all-garnet multilayer structures, applying oxygen plasma treatment on amorphous garnet layers just after the deposition process, and designing modifications of the annealing crystallization process and regimes for achieving the best MO properties. We demonstrated significant improvement in MO properties of Bi-containing ferrite-type garnet thin-film materials, including record-high MO figures of merit and improved conventional and un-conventional hysteresis loops of Faraday rotation. The attractive optical, magnetic, and magneto-optic properties obtained in highly bismuth-substituted iron garnet thin-film materials of multiple composition types are relevant in the context of manufacturing next-generation ultra-fast optoelectronic devices, such as light intensity switches and modulators, high-speed flat panel displays, and high-sensitivity sensors.