Solid particle erosion (SPE) tests are carried out to evaluate the performance of plasma sprayed coatings of borosilicate glass microspheres (BGM) premixed with Al2O3 particles on metallic substrates. For this purpose, an Air Jet Erosion test rig confirming to ASTM G 76 test standards is used. Relative influence of different operating parameters on erosion rate is assessed by statistical analysis of the experimental findings that are based on Taguchi’s L16 orthogonal array. This analysis helps to identify the most significant factor affecting the erosion wear rate of the coating. The study reveals that the impact velocity, impingement angle, erodent size, and Al2O3 content in the feed stock, in the declining sequence, are the significant factors influencing the wear rate of these coatings. An Artificial Neural Network (ANN) approach is then implemented taking into account training and test procedure to predict the triboperformance of these coatings under wear conditions beyond the experimental range. Further, the microstructural features of the eroded samples are studied from SEM images to identify possible wear mechanisms.