The crystal structure, lattice dynamics and themomechanical properties of bulk monoclinic zirconium tetrachloride (ZrCl4) have been investigated using zero-damping dispersion-corrected density functional theory [DFT-D3(zero)]. Phonon analysis reveals that ZrCl4(cr) undergoes negative thermal expansion (NTE) near T approximate to 10 K, with a coefficient of thermal expansion of alpha = -1.2 ppm K-1 and a Gruneisen parameter of gamma = -1.1. The bulk modulus is predicted to vary from K-0 = 8.7 to 7.0 GPa in the temperature range 0-550 K. The isobaric molar heat capacity derived from phonon calculations within the quasi-harmonic approximation is in fair agreement with existing calorimetric data. (C) 2017 Elsevier B.V. All rights reserved.