The Raman spectrum of vanadium tetrachloride has been recorded in carbon tetrachloride; the values for the four fundamentals are ν1(a1) 385, ν2(e) 111, ν3(t2) 483, ν4(t2) 128 cm–1. Values for the force constants and thermodynamic parameters of vanadium tetrachloride have been obtained. Raman intensity measurements on the a1 band by use of the 6471, 5682, 5308 and 5208 Å exciting lines of the krypton ion laser indicate considerable resonance enhancement to its intensity as the frequency of the exciting line approaches that of the first allowed electronic transition of the molecule. The vanadium-chlorine bond polarisability derivative, text-decoration:overlineα′VCl, obtained by extrapolation to zero exciting frequency, is 4.00 Å2.