Heavy-duty diesel engines are essential mechanic power generation tools for industry and transporting freight and passengers. Therefore, increasing engine efficiency and minimizing maintenance and repair costs is crucial. This study examines and characterizes three thermal spray coatings (Cr3C2/NiCr, NiCr, and Al2O3/TiO2) utilized on cylindrical gray cast iron substrate specimens. The coatings were tested for their microstructural (optical microstructure, SEM, EDS, XRD, and AFM topography), mechanical (nanoindentation and nano scratch), and tribological (short and long-distance wear test) properties. Microstructural tests showed that an average coating thickness of 120 to 170 µm was successfully achieved on the cast iron base substrate using different thermal coating methods. The Cr3C2/NiCr coating, observed through the AFM mapping method, achieved the most uniform roughness distribution on the surface. The elasticity of the coatings was measured with a nanoindentation test, and Al2O3/TiO2 coating exhibited high rigidness (177 GPa). The nano scratch test showed that the highest load-carrying capacity was achieved with the Cr3C2/NiCr coated sample. NiCr-coated sample exhibited approximately similar rigidness (61 GPa) to cast iron (67 GPa). Short- and long-distance wear tests showed that the coatings provided significantly better wear resistance than the cast iron base. The coatings’ efficacy was evident. At the long-distance tests, while the cast iron base sample had a wear rate of 19.874 (10−7mm3/Nm), the wear rates of Al2O3/TiO2, Cr3C2/NiCr, and NiCr coatings were 3.835, 4.020, and 6.466 (10−7mm3/Nm), respectively. The Al2O3/TiO2 and Cr3C2/NiCr coatings had superior tribological performance than the NiCr coating, yet the NiCr coating showed much higher wear performance than the uncoated base. The Cr3C2/NiCr coating exhibited superior tribomechanical performance in all the coatings.