A Raman spectroscopy-based step-by-step measuring method of Euler angles φ, θ, and ψ was presented for the wurtzitic crystal orientation on a microscopic scale. Based on the polarization selection rule and coordinate transformation theory, a series of analytic expressions for the Euler angle measurement using Raman spectroscopy were derived. Specific experimental measurement processes were presented, and the measurement of Raman tensor elements and Euler angles of the ZnO crystal were implemented. It is deduced that there is a trigonometric functional relationship between the intensity of each Raman bands of wurtzite crystal and Euler angle ψ, the polarization direction of incident light under different polarization configurations, which can be used to measure the Euler angles. The experimental results show that the proposed method can realize the measurement of Euler angles for wurtzite crystal effectively.