High-intensity pulsed ion beam (HIPIB) irradiation at 300 A/cm2 with a shot number of 1, and 5 was performed on the coatings and caused the modification of properties. Porosity and rough surface of EB-PVD (Electron Beam-Physical Vapor Deposition) deposited ZrO2-7%Y2O3 coatings with the thickness of 150 μm on heat-resistant steel have been characterized using the ultrasonic reflection coefficient phase spectrum. With increasing the shot number, the surface remelting and ablating filled gaps and caves between columns, and induced more uniform and compact structure. The ultrasonic measurement was investigated using immersion focusing pulse echo method with a 10 MHz transducer. The ultrasonic reflection coefficient related to frequency, velocity and attenuation coefficient were analyzed based on the acoustic transmission model in a multi-layered structure. For the as-deposited coating and coatings irradiated by HIPIB with the shot number of 1 and 5, the ultrasonic velocity changed from 2950 to 3170, and 3255 m/s respectively. The relationship between the attenuation coefficient and the frequency has been deduced based on the numerical fitting of the phase spectrum. The corresponded expressions are 1.35 α = 0.105 f , 1.2 α = 0.045 f and 1.14 α = 0.035 f , which displays that the attenuation coefficient decreases with the increasing of shot number. The ultrasonic results are in agreement with SEM observations, which have indicated that the coatings became denser and uniform with increasing the shot number. From the velocity and attenuation coefficient, the density, porosity, and microcracks of the coatings can be nondestructively evaluated utilizing the method of this paper.