The Raman spectra of a lithium tantalate crystal doubly doped with chromium and neodymium LiTaO3:Cr(0.2):Nd(0.45 wt%) have been studied in this paper. Raman spectra of the first and second orders have been found to be located against the background of a luminescent halo with a maximum at ≈1250 cm−1. Several Raman bands have been detected in the frequency range of 900–2000 cm−1. Their frequencies were 940, 1034, 1113, 1171, 1250, 1343, 1428, 1491, 1582, 1735, 1838, and 1925 cm−1. These bands correspond to overtone processes. We have determined that the frequencies of 1838 and 1925 cm−1 bands are significantly higher than the exact value of the overtone frequency corresponding to the fundamental mode 4A1(z)LO (864 cm−1).