Galvannealed steels are produced by reheating of Zinc-coated steels, in which the iron and the zinc are interdiffused to form Zn-Fe intermatallic compound. In recent years, application of galvannealed steel has increased due to its excellent corrosion resistance, good weldability and paintability. Galvannealed production requires strict control of processing conditions to obtain an optimal alloying degree in the coatings. The analysis of the alloying degree is very important since they are closely related to the corrosion and mechanical properties. This study is measurement of alloying degree of the galvannealed steel by using the XRD. Partial least squares (PLS) model is a powerful multivariate tool that has been successfully applied to the quantitative analysis of data in XRD. The alloying degree was determined by using PLS regression to a concentration accuracy of 0.2%. The XRD analysis and proposed PLS model can be successfully used to determine the alloying degree of industrially produced galvannealed steel.