Ni-Cr thin films with chromium concentrations spanning the 0-100% range were coevaporated onto NaCl substrates held at room temperature, 200 and 300 degrees C. Analytical transmission electron microscopy provided complete identification of the phases present in the films and characterization of their microstructures. Films of 0-40% Cr contained grains of the f.c.c. solid solution of chromium in nickel which, when formed at 200 or 300 degrees C, exhibited {111}[11 $$($) over bar 2] twinning. Films of 50-70% Cr deposited onto room temperature substrates contained nanocrystalline sigma phase, while larger grains of sigma phase were found for elevated substrate temperature depositions. Films of 80% Cr, deposited onto 300 degrees C substrates, contained delta phase with the A15 structure in addition to the b.c.c. solid solution of nickel in chromium observed in films deposited onto lower temperature substrates. These observations are discussed in terms of thermodynamic calculations and electron phase considerations as they apply to the Ni-Cr alloy system.