Atmospheric plasma spraying (APS) is a most versatile thermal spray method for depositing alumina (Al2O3) coatings, and detonation gun (D-gun) spraying is an alternative thermal spray technology for depositing such coatings with extremely good wear characteristics. The present study is aimed at comparing the characteristics of Al2O3 coatings deposited using the above techniques by using Taguchi experimental design. Alumina coating experiments were conducted using a Taguchi fractional-factorial (L8) design parametric study to optimize the spray process parameters for both APS and D-gun. The Taguchi design evaluated the effect of four APS and D-gun spray variables on the measured coating attributes. The coating qualities evaluated were surface roughness, porosity, microhardness, abrasion, and sliding wear. The results show that the coating quality is directly related to the corresponding coating microstructure, which is significantly influenced by the spray parameters employed. Though it is evident that the D-gun-sprayed coatings consistently exhibit dense and uniform microstructure, higher hardness, and superior tribological performance, the attainment of suitable plasma-sprayed coatings can be improved by employing the Taguchi analysis.