The characterization of zirconium hydride is important in the nuclear industry because of the hydrogen-induced embrittlement of Zircaloy cladding and its use as a neutron moderator. This paper introduces the use of Raman spectroscopy for the characterization of zirconium hydride. First-principles density functional theory (DFT) calculations were used to predict the Raman spectra of ζ-ZrH0.5, γ-ZrH, δ-ZrH1.5, δ-ZrH1.66, and ε-ZrH2 with all their predicted symmetries; ζ-ZrH0.5 (P3m1, R3¯m, C2/m, Cm, Cmmm, and Pn3¯m); γ-ZrH (P222, Ccce, and P42/mmc); δ-ZrH1.5 (P4¯m2, P42/mcm, Fmmm, Pn3¯m, Ibam, P2/c, PI, and P42/nnm); δ-ZrH1.66 (Fm3¯m); and ε-ZrH2 (Fm3¯m, R3¯m, and I4/mmm). Two samples of Zircaloy-4 containing 133 wt ppm and 360 wt ppm hydrogen were characterized by Raman spectroscopy, showing two signal lines at 215 cm−1 and 1,187 cm−1, which were assigned to the presence of δ-ZrH1.66. These signals had a good spatial correlation with visible hydride precipitates in Raman spectroscopy images. This work provides the basis for the characterization of all possible zirconium hydride compositions and structures using Raman spectroscopy.