This paper describes the simultaneous determination of the ultrasonic parameters in thermally sprayed coatings. The parameters of interest are the longitudinal wave velocity and the ultrasonic attenuation. The test materials are two cobalt-based coatings (FSX 414 and Diamalloy 4060), both deposited onto stainless steel (310SS) substrates. The ultrasonic measurements were carried out in the pulse-echo configuration using several transducers. The ultrasonic signals reflected from the coatings were successfully estimated using the combined model, together with the maximum likelihood estimation and the Levenberg–Marquardt approach. The best estimate was obtained for 20 MHz measurements. Once the model was validated, the ultrasonic parameters of the thermally sprayed coatings were extracted. Model validation is based on the analysis of the residual between measured and estimated signals. Results showed non-dispersive ultrasonic velocities with average values of (3940±50)m/s" role="presentation" style="box-sizing: border-box; display: inline-table; line-height: normal; letter-spacing: normal; word-spacing: normal; overflow-wrap: normal; white-space: nowrap; float: none; direction: ltr; max-width: none; max-height: none; min-width: 0px; min-height: 0px; border: 0px; padding: 0px; margin: 0px; position: relative;">(3940±50)m/s(3940±50)m/s in Diamalloy 4060 and (4260±20)m/s" role="presentation" style="box-sizing: border-box; display: inline-table; line-height: normal; letter-spacing: normal; word-spacing: normal; overflow-wrap: normal; white-space: nowrap; float: none; direction: ltr; max-width: none; max-height: none; min-width: 0px; min-height: 0px; border: 0px; padding: 0px; margin: 0px; position: relative;">(4260±20)m/s(4260±20)m/s in FSX 414. High ultrasonic attenuation with a quadratic frequency dependence was observed for both materials. Moreover, it was found that the ultrasonic parameters in thermally sprayed materials are microstructure dependent. For close densities, the harder the coating, the higher the ultrasonic wave velocity and attenuation.