Manufacturing of alloyed cast iron forming rolls is accompanied by generation of valuable solid waste as cutting and grinding swarf. The objective of this investigation was to evaluate the potential for mill debris to be used as a new source of inexpensive powders for thermal spraying of wear resistant coatings. More than 25 high-carbon iron alloy compositions are used in roll production. The structure of these cast irons usually includes from 2 to 4 phases (such as troostite, bainite, needled martensite, austenite, and graphite). The properties of powders obtained from mill debris were characterized in terms of particle size and shape, composition, structure, technological fluidity, and bulk density. The obtained powders were used for plasma spraying of wear resistant coatings. The results indicate that cutting and grinding swarf may be a feasible raw material source for economical alloyed powders, granules, and other materials for coatings. The composite plasma sprayed coatings obtained from powder mixtures of alloyed cast iron and nickel-base alloy have better tribological performance in comparison to coatings from any single powder alloy.