We report high-precision magnetization (), magnetic susceptibility (), specific heat (Cp (T, H)) and ‘zero-field’ electrical resistivity, , data taken on Gd2Te3 single crystal over wide ranges of temperature and magnetic field (H), with either -axis or -plane. and unambiguously establish that the b-axis is the easy direction of magnetization whereas any direction in the ac-plane is a hard direction. The -type anomaly in ‘zero-field’ specific heat, Cp (T, H = 0), and an abrupt drop in (characteristic of the paramagnetic (PM) — antiferromagnetic (AFM) phase transition) are observed at the Néel temperature, K. and Cp (T,H) clearly demonstrate that shifts to lower temperatures with increasing H irrespective of whether H points in the easy or hard direction. When , the isotherms at temperatures in the range 2.5 K K reveal the existence of a field-induced spin-flop (SF) transition at fields 4.0 T 4.5 T. The first principles electronic band structure and density of states calculations, based on the density functional theory, correctly predict an AFM ground state (stabilized primarily by the 4f Gd3+ – 5p Te2−– 4f Gd3+ superexchange interactions) and the observed semi-metallic behavior for the Gd2Te3 compound. Moreover, these calculations yield the values for the ordered magnetic moment per Gd atom at T = 0, mJ mol−1 K−2 for the Sommerfeld coefficient for the electronic specific heat contribution and K for the Curie–Weiss temperature, respectively. These theoretical estimates conform well with the corresponding experimental values , mJ mol−1 K−2 and K.