The preparation of coatings by atmospheric plasma spraying gives rise to complex physical processes, which present challenges to the study of plasma jet characteristics and particle in‐flight behavior. Herein, a 3D numerical model that integrates multiple physical phenomena, including electromagnetism and thermal and gas dynamics, to simulate the heating, acceleration, and melting of particles under the thermal–mechanical effect, is developed. Meanwhile, yttria‐stabilized zirconia (YSZ) coatings are prepared under varying process parameters. The DPV‐2000 system is employed for the diagnosis of particle velocity, surface temperature, and diameter. Following comparison, the simulation exhibits errors of 4.5% and 14.8% for the maximum temperature and velocity, respectively. An increase in current intensity from 500 to 600 A results in a rise in the proportion of particles exhibiting temperatures above the melting point (2963 K), from 75.1 to 93.4%, accompanied by an increase in average velocity of ≈16.6%. As the spraying distance increases from 60 to 100 mm, the proportion of particles melting decreases from 93.5 to 66.3%, and the average velocity decreases by ≈9.2%. This work will provide a theoretical foundation for the optimization of process parameters to adjust particle behavior and melting state, thus achieving an optimal spraying effect.