We report on the development of several different thin-film functional material systems prepared by radio frequency (RF) magnetron sputtering at Edith Cowan University nanofabrication labs. While focusing on the RF sputtering process optimizations for new or the previously underexplored material compositions and multilayer structures, we disclose several unforeseen material properties and behaviours. Among these are an unconventional magnetic hysteresis loop with an intermediate saturation state observed in garnet trilayers, and an ultrasensitive magnetic switching behaviour in garnet-oxide composites (GOC). We also report on the unusually high thermal exposure stability observed in some nanoengineered metal–dielectric multilayers. We communicate research results related to the design, prototyping, and practical fabrication of high-performance magneto-optic (MO) materials, oxide-based sensor components, and heat regulation coatings for advanced construction and solar windows.