Nondestructive techniques for evaluating and characterizing coatings have been extensively demanded by the thermal spray community; nonetheless, few results have been produced in practice due to difficulties in analyzing the complex structure of thermal spray coatings. Of particular interest is knowledge of the elastic modulus values and Poisson’s ratios, which are very important when seeking to understand and/or model the mechanical behavior or develop life prediction models of thermal spray coatings employed in various applications (e.g., wear, fatigue and high temperatures (TBCs)). In the present study, two techniques, laser-ultrasonics and Knoop indentation, were used to determine the elastic modulus of thermal spray coatings. Laser ultrasonics is a non-contact and nondestructive evaluation method that uses lasers to generate and detect ultrasound. Ultrasonic velocities in a material are directly related to its elastic modulus value. The Knoop indentation technique, which has been widely used as a method for determining elastic modulus values, was employed in order to compare and validate the measurements of the laser-ultrasonic technique. The determination of elastic modulus values via the Knoop indentation technique is based on the measurement of elastic recovery of the dimensions of the Knoop indentation impression. The approach used in the present study was to focus on evaluating the elastic modulus of very uniform, dense and near-isotropic titania and WC-Co thermal spray coatings using these two techniques. Four different coatings were evaluated: two titania coatings produced by APS and HVOF and two types of WC-Co coatings, conventional and multimodal (nanostructured and micro-sized particles), deposited by HVOF.