This invention relates to thermally sprayed coatings having an amorphous-nanocrystalline-microcrystalline composition structure, said thermally sprayed coating comprising from about 1 to about 95 volume percent of an amorphous phase, from about 1 to about 80 volume percent of a nanocrystalline phase, and from about 1 to about 90 volume percent of a microcrystalline phase, and wherein said amorphous phase, nanocrystalline phase and microcrystalline phase comprise about 100 volume percent of said thermally sprayed coating. This invention also relates to methods for producing the coatings, thermal spray processes for producing the coatings, and articles coated with the coatings. The thermally sprayed coatings of this invention provide enhanced wear and corrosion resistance for articles used in severe environments (e.g., landing gears, airframes, ball valves, gate valves (gates and seats), pot rolls, and work rolls for paper processing).