Electrodeposition of Ni 1-x Fe x (x = 0.1-0.9) films was carried out from a chloride plating solution containing saccharin as an organic additive at a constant current density (5 mA/cm 2 ) and a controlled pH of 2.5. X-ray diffraction studies revealed the existence of an fcc, or ␥ phase, in the range of 10-58 wt.% Fe, a mixed fcc/bcc phase in the range of 59-60 wt.% Fe, and a bcc, or ␣ phase in the range of 64-90 wt.% Fe. The saturation magnetization, B s , of electrodeposited Ni 1-x Fe x alloys at the room temperature was found to increase with the increase of Fe-content and follows the Slater-Pauling curve, but deviates from as-cast bulk NiFe alloys. The coefficient of thermal expansion, CTE, of electrodeposited alloys at room temperature also deviates from as-cast bulk NiFe alloys. Annealing of ␣-Ni 36 Fe 64 alloy results in a martensitic ␣ → ␥ phase transformation, which takes place between 300 and 400 • C. It was demonstrated that thermal treatment above 400 • C was necessary to obtain magnetic and mechanical properties similar to those to conventional Invar alloy. Annealing of ␣-Ni 36 Fe 64 alloy at 700 • C brings about a decrease of B s from 1.75 to 0.45 T. By controlling the annealing conditions of ␣ → ␥ martensitic transformation, it is possible to adjust the CTE of Ni 36 Fe 64 alloy over the broad limits from 2.7 to 8.7 × 10 -6 / • C.