The structural and vibrational properties of lithium niobate (LN) -lithium tantalate (LT) mixed crystals (LNT, LiNb 1-x Ta x O 3 ) are investigated over the whole composition range by first-principles simulations. The crystal volume grows roughly linearly from LT to LN, whereby the lattice parameters a and c show minor deviations from the Vegard behavior between the end-compounds, LiNbO 3 and LiTaO 3 . Our calculations in the framework of the density functional theory show the TO 1 , TO 2and TO 4 -modes to become harder with increasing Nb concentration. TO 3 becomes softer with increasing Nb content, instead. The frequency shifts of the zone center A 1 -TO phonon modes for crystals with different compositions are found to be as large as 30 cm -1 . Raman spectroscopy, which is sensitive to the A 1 modes, can be therefore employed to determine the crystal composition.