Thickness is a very important parameter with which to control the microstructures, along with physical properties in transition-metal nitride thin films. In work presented here, CrN films with different thicknesses (from 26 to 130 nm) were grown by chemical solution deposition. The films are pure phase and polycrystalline. Thickness dependence of microstructures and electrical transport behavior were studied. With the increase of films thickness, grain size and nitrogen content are increased, while resistivity, zero-field sensitivity and magnetoresistance are decreased. In the temperature range of 5–350 K, all samples exhibited semiconductor-like properties with dρ/dT < 0. For the range above and below the Néel temperature, the resistivity can be fitted by the thermal activation model and the two-dimensional weak localization (2D-WL) model, respectively. The ultra-low magnetoresistance at a low temperature under high magnetic fields with a large zero-field sensitivity was observed in the CrN thin films. The zero-field sensitivity can be effectively tuned to 10−2 K−1 at 5 K with a magnetoresistance of less than 1% at 2 K under 14 T by reasonably controlling the thickness.