This study examines microstructural-based mechanical properties of Al-Cu composite deposited by cold spraying and wire arc sprayed nickel-based Alloy 625 coating using numerical modeling and experimental techniques. The microhardness and elastic modulus of samples were determined using the Knoop hardness technique. Hardness in both transverse and longitudinal directions on the sample cross-sections has been measured. An image-based finite element simulation algorithm was employed to determine the mechanical properties through an inverse analysis. In addition mechanical tests including, tensile, bending, and nano-indentation tests were performed on Alloy 625 wire arc sprayed samples. Overall, results from the experimental tests are in relatively good agreement for deposited Al-Cu composites and Alloy 625 coating. However, results obtained from numerical simulation are significantly higher in value than experimentally obtained results. Examination and comparison of the results are strong indications of the influence of microstructure characteristics on the mechanical properties of thermally spray deposited coatings.