Deposition of (Ti-Al)N/MoN multilayered coatings was carried out through a cathodic ion-plating system in an argon and then nitrogen atmosphere. Bilayer thickness (Λ) of all the samples were achieved, from 22 to 104 nm, by organizing substrate holder rotational speed (SRS). To obtain the optimum properties of the (Ti-Al)N/MoN coatings, the Ti and Al ratio was maintained at a level of 1:1. X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), X-ray photoelectron spectroscopy (XPS), and Raman spectroscopy were utilized to analyze the crystal structure and morphology of the coatings. Mechanical and tribological properties were examined by nanohardness and atomic force microscopy (AFM). The preferred orientation of the (Ti-Al)N/MoN nanoscale multilayer films was TiAlN (200) and MoN (200), which had face centered cubic (fcc) and hexagonal structures, respectively. The hardness increased with the decrease in Λ (104 nm to 26 nm), and then it increased. The highest hardness of 37 GPa was revealed at Λ = 26 nm, whereas the least wear rate of 8.09 × 10−7 mm3/N.m was attained at Λ = 22 nm. Wear rate, roughness, and coefficient of friction were decreased with decreasing bilayer period. EDS results showed that Al and Ti contents were almost the same in all samples, as per design of the experiment.