The characterization of thermal-sprayed coatings is often limited to microstructural analysis to evaluate the coatings morphology. Indentation is commonly used to determine the mechanical properties of different kinds of engineering materials. However, due to the complex structure of thermal-sprayed coatings, few results have been obtained so far. In this article, experimental nanoindentation tests and simulation results are compared. The experimental indentation tests show scattering in the force-deformation data due to the complex structure of the arc-sprayed coating which is investigated by means of an indentation test simulation. Based on the results for single constituent parts of the coating, the Young's modulus as well as further mechanical properties are identified. A general procedure is presented to predict the effective mechanical properties based on the microstructure, porosity, chemical composition, and properties of the coating after thermal spraying.