Various natural materials, namely ilmenite, diopside, tourmaline, olivine, garnet, and basalt, were plasma-sprayed and analyzed. This paper summarizes the various achievements of our earlier research and adds new results—mainly dielectric and optical characterizations. Plasma spraying of all of the materials was rather easy with a high feed-rate plasma system, which could process many kilograms of powder per hour. For easier characterizations, the coatings were detached from substrates in order to remain self-supporting. The plasma-sprayed layers that were coated from all studied materials acted as medium-permittivity and low-loss dielectrics, antireflective optical materials, and medium quality anti-abrasive barriers. Phase composition and microhardness were evaluated in addition to microstructure observations. Some coatings were amorphous and crystallized after further heating. As the melting points were well above 1000 °C, all of them could also serve as thermal barriers for aluminum alloys and similar metals. The only material that was not easily sprayed was tourmaline, which gave very porous coatings without environmental barrier or dielectric characteristics.