The primary purpose of grit blasting for thermal spray applications is to ensure a strong mechanical bond between the substrate and the coating by the enhanced roughening of the substrate material. This study presents statistically designed experiments that were accomplished to investigate the effect of abrasives on roughness for A36/1020 steel. The experiments were conducted using a Box statistical design of experiment (SDE) approach. Three grit blasting parameters and their effect on the resultant substrate roughness were investigated. These include blast media, blast pressure, and working distance. The substrates were characterized for roughness using surface profilometry. These attributes were correlated with the changes in operating parameters. Twin-Wire Electric Arc (TWEA) coatings of aluminum and zinc/aluminum were deposited on the grit-blasted substrates. These coatings were then tested for bond strength. Bond strength studies were conducted utilizing a portable adhesion tester following ASTM standard D4541.