The growth, structural, and electrical characterization of vacuum‐deposited n‐ and p‐type CuInTe2 thin films utilizing a high‐evaporation‐rate technique (≳100 Å/s) are reported. Complementary transmission electron microscopy (TEM) and Auger electron spectroscopy (AES) are used to investigate the films’ crystalline (grain size, orientation, structure) and compositional (elemental) properties. The effects of substrate temperature on these quantities are presented. A substrate temperature range (400<Tsub<525 K) has been identified for the growth of single phase, chalcopyrite CuInTe2 thin films which have a preferred (112) orientation. Selected area diffraction and Auger analyses have detected Te inclusions at low Tsub and In inclusions for Tsub≳525 K. Annealing of the films in argon is used to increase grain size from ∠1000 Å for as‐deposited films to the 2000–6000 Å range. The as‐deposited films have characteristically high resistivities, in excess of 103 Ω cm. The effects of a low‐temperature (673 K) annealing procedure on the films’ electrical characteristics are indicated and are correlated with the corresponding structural changes. The temperature dependences of the mobilities, conductivities, and carrier concentrations of both n‐ and p‐type annealed films are presented and explained in terms of a grain‐boundary scattering mechanism. Film mobilities, μn∠20–30 cm2 V−1 s−1 and μp∠5–12 cm2 V−1 s−1 have been measured. The majority‐carrier type is found to depend on Tsub for these vacuum‐deposited ternary films, and a range, 443<Tsub<463 K, has been identified over which the change from n (lower Tsub) to p (higher Tsub) occurs.