Ni80Fe20/Ni48Fe12Cr40 bilayer films and Ni80Fe20 monolayer films were deposited at room temperature on SiO2/Si(100) substrates by electron beam evaporation. The influence of the thickness of the Ni48Fe12Cr40underlayer on the structure, magnetization, and magnetoresistance of the Ni80Fe20/Ni48Fe12Cr40 bilayer film was investigated. The thickness of the Ni48Fe12Cr40 layer varied from about 1 nm to 18 nm while the Ni80Fe20 layer thickness was fixed at 45 nm. For the as-deposited bilayer films the introducing of the Ni48Fe12Cr40 underlayer promotes both the (111) texture and grain growth in the Ni80Fe20 layer. The Ni48Fe12Cr40 underlayer has no significant influence on the magnetic moment of the Ni80Fe20/Ni48Fe12Cr40 bilayer film. However, the coercivity of the bilayer film changes with the thickness of the Ni48Fe12Cr40underlayer. The optimum thickness of the Ni48Fe12Cr40 underlayer for improving the anisotropic magnetoresistance effect of the Ni80Fe20/Ni48Fe12Cr40 bilayer film is about 5 nm. With a decrease in temperature from 300 K to 81 K, the anisotropic magnetoresistance ratio of the Ni80Fe20 (45 nm)/Ni48Fe12Cr40 (5 nm) bilayer film increases linearly from 2.1% to 4.8% compared with that of the Ni80Fe20 monolayer film from 1.7% to 4.0%.