The complex electronic properties of ZrTe5 have recently stimulated in-depth investigations that assigned this material to either a topological insulator or a 3D Dirac semimetal phase. Here we report a comprehensive experimental and theoretical study of both electronic and structural properties of ZrTe5, revealing that the bulk material is a strong topological insulator (STI). By means of angle-resolved photoelectron spectroscopy, we identify at the top of the valence band both a surface and a bulk state. The dispersion of these bands is well captured by ab initio calculations for the STI case, for the specific interlayer distance measured in our x-ray diffraction study. Furthermore, these findings are supported by scanning tunneling spectroscopy revealing the metallic character of the sample surface, thus confirming the strong topological nature of ZrTe5.The discovery of topological insulators (TIs), characterized by metallic spin-polarized surface states connecting the bulk valence and conduction bands [1], has stimulated the search for novel topological phases of matter [2][3][4][5][6]. ZrTe 5 has recently emerged as a challenging system with unique, albeit poorly understood, electronic properties [7][8][9][10][11][12][13][14][15][16][17]. Magneto-transport [11], magneto-infrared [13] and optical spectroscopy [14] studies describe ZrTe 5 in terms of a 3D Dirac semimetal. Theoretical calculations have predicted its bulk electronic properties to lie in proximity of a topological phase transition between a strong and a weak TI (STI and WTI, respectively), where only the former displays topologically protected surface states at the experimentally accessible (010) surface [10]. The monolayer is also computed to be a 2D TI [10] and scanning tunneling microscopy/spectroscopy (STM/STS) experiments suggest the existence of topologically protected states at step edges [18,19]. However, the unambiguous identification of the topological phase of ZrTe 5 is still lacking.In this Letter we report on the STI character of the bulk ZrTe 5 by combining ab initio calculations and multiple experimental techniques, at temperature both above and below the one of the resistivity peak, T * ∼ 160 K [7][8][9]15]. Angleresolved photoelectron spectroscopy (ARPES) experiments in the ultraviolet (UV) and soft x-ray (SX) energy ranges reveal the presence of two distinct states at the top of the valence band (VB). On the basis of photon energy dependent studies, we ascribe the origin of these two states to the bulk and crystal surface, respectively. We have performed ab initio calculations of the topological phase diagram of ZrTe 5 , as a function of the interlayer distance b/2. Our measured band dispersion is in agreement with the calculations and it is consistent with the STI case for b/2 = 7.23 ± 0.02Å. This value has been confirmed for our specimen by x-ray diffraction (XRD) measurements. Furthermore, the 3D Dirac semimetal phase is not protected by crystalline symmetries, and it manifests only for the specific b/2 = 7.35Å at the boundar...