The use of phase-Doppler anemometry (PDA) to characterize the detail in-flight plasma sprayed particle behavior has been demonstrated previously [Ma et al. Plasma Chem Plasma Process 24(1):85; 25(1):56] The present articles shows further that a direct relationship may exist between the PDA measured particle volume flux and the coating microstructure and deposition efficiency (DE). In the situation when the precise particle temperature information is not available, the PDA measured particle volume flux may provide an alternative to predict quantitatively the variation of the coating microstructure and the DE. By monitoring the in-flight particle volume flux variations, instead of the particle velocity, size and temperature individually and simultaneously, the optimal settings of the plasma spraying parameters may also be determined conveniently. However, it is noted that the effective applications of such approach depend largely on the particle surface morphology and the pre-determination of the particle size range.