Nanostructured TiCrN films were grown on Si (100) wafers by reactive DC unbalanced magnetron cosputtering technique without external heating and voltage biasing to the substrates. The effects of Ti sputtering current on the chemical composition, chemical state, electronic structure, crystal structure, and morphology of the TiCrN films were characterized by X-ray photoelectron spectroscopy (XPS), X-ray diffraction (XRD), atomic force microscopy (AFM), and field emission scanning electron microscopy (FE-SEM), respectively. The results showed that all prepared films were formed as an understoichiometric (Ti, Cr)N solid solution with the fcc B1 type phase. The films exhibited a nanostructure with a crystallite size of less than 14 nm. The deconvolution of XPS spectra revealed the chemical bonding between Ti, Cr, N, and O elements. The addition of Ti contents led to the decrease of valence electrons filled in the d conduction bands which result in the change of binding energy of electrons in core levels. The roughness of the films was found to increase with increasingITi. The cross-sectional morphology of the films showed columnar structure with dome tops.