In this work, four series of glass-ceramic coatings were developed and applied by using the dipping technique to cast iron sheets. The influence of different types of crystallization agents (Li2O, TiO2, ZrSiO4, and CaO.Al2O3.2SiO2) was investigated in relation to the mechanical features of the coatings. The resultant coating is characterized using X-ray diffraction analysis. The properties of micro-hardness and adhesion strength are evaluated using suitable standard tests. The X-ray analysis of resultant coatings showed the existence of some of crystalline phases formed depending on the type of the crystallization agent. The results also indicated that the coating properties were strongly dependent on composition and concentration of crystallization agent. Coating with feldspar gives the highest value of hardness and adhesion index. In general, properties of the resultant coatings were improved in all cases; this is related to the formation of a complicated network from crystalline phases.