CrO2–Al2O3 composite films were deposited on Si(100) substrates by the atmospheric pressure chemical vapor deposition method using CrO3 and AlBr3 as precursors. The CrO2–Al2O3 composite films consist of large CrO2 grains and Al2O3 nanoparticles. The composition of the films was controlled by adjusting the temperature of CrO3 during deposition. The CrO2–Al2O3 composite film with Al2O3 content of 0.38 (molar fraction) shows insulator–metal transition. Below 120K, it is insulator and the temperature dependence of its resistance can be well explained by the fluctuation-induced tunneling model; above 175K, it is metallic. It shows large intergrain tunneling magnetoresistance at low temperature, which reaches −15.2% at 5K and 50kOe. While at high temperature the intergrain tunneling magnetoresistance in the film nearly disappears, and the film shows a small linear magnetoresistance, which should be due to the double-exchange mechanism in CrO2.