Raman spectra of oriented single crystals of NaBF, were measured at 77 and 298 K. The number of bands and the intensities were in excellent agreement with the unit cell group predictions for the known crystal structure, Di2, Z = 2. The results for the vl, v2 and v, regions were in excellent agreement with those of Bates [ J . Ckm. Phys. 55, 489 (1971)l. A recent study by Rajakumar et al. [J. Ramm Spectrosc. 23, 75 (1992)l is erroneous. The new measurements permitted the assignment for the Raman bands in the vj region. Peaks in the external mode region were very weak because both the Na' and BF,-ions have spherical symmetry, small polarizabilities and small polarizability derivatives with respect to normal coordinates. Only three weak peaks of the nine predicted externalmodes were observed (88 cm-', A,; 110 cm-', &; and 214 cm-', B2,). Crystals grown from aqueous solution were found to contain water and as much as 0.1% of BF,OH-as a substitutional impurity. Peaks due to the 0-H (0-D) stretching vibration were detected in the crystals at 3641 (2688) cm-' and peaks due to the B-OH (BOD) stretching vibration were detected as 773 (748) cm-'.