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The aim of this work is to investigate the possibility of improving the performance properties of 40CrMnMo7 steel by conducting duplex surface modification treatment. Chemical-thermal treatment processes were used—nitrocarburization and ion-nitriding and subsequent application of a nanostructured multilayer coating, Cr/(Cr-C)ml. The resulting structures and their influence on the adhesion of the applied coating, as well as their influence on the tribological properties of the coating, were studied. By conducting Glow Discharge Optical Emission Spectroscopy (GDOES), it was established that the penetration of nitrogen into the depth is greater in the ion-nitriding process, and the results of the conducted optical metallography and hardness measurement show that after ion-nitriding, the obtained hard layer has a greater thickness and hardness. The data obtained from the studies of the phase composition of the hard layers show that after nitrocarburization the non-stoichiometric, but crystalline phase Fe3N1.1 (ξ)—98.4% was formed. In the composition of the hard layer formed after the ion-nitriding process, the presence of Fe3N (ξ-phase) in an amount of 79.5% and Fe4N (γ′-phase) in an amount of 19.1% was established. On the chemically and thermally treated surfaces, a Cr/(Cr-C)ml coating was applied through the unbalanced magnetron sputtering technology. The applied coating has a hardness of 17.1 ± 0.6 GPa and a modulus of elasticity of 289 ± 8.7 GPa. The thickness of the coating applied on the test bodies not subjected to diffusion enrichment is 1.967 µm, and the adhesion class is classified as HF-2. It has been established that the profile of the surfaces obtained after the application of the chemical-thermal treatment processes has an impact on the thickness of the applied coating and on its adhesion. After nitrocarburization, the thickness of the coating is 2.9 µm, and the adhesion of the coating is classified as HF-0. The thickness of the applied coating on the test bodies subjected to ion-nitriding is 2.4 µm, and the adhesion class is HF-1. The results of the conducted tribological tests show that the used chemical-thermal treatment processes have an impact on the coefficients of friction and wear of the coating. The coefficient of friction for the combination of the nitriding process and Cr/(Cr-C)ml coating has the highest value (µ ≈ 0.38), while that of the ion-nitrided sample with subsequent coating has a value (µ ≈ 0.21) slightly higher than the COF of the test body with only the coating applied (µ ≈ 0.18). The lowest value of the coating wear coefficient is registered for the combination of the ion-nitriding and coating process (k = 7.96 × 10−5), while for the combination of nitriding and coating, it is the highest (k = 12.4 × 10−4). The relevance of the present work is related to the implementation of surface modification of 40CrMnMo7 steel by using established technological processes of chemical-thermal treatment and subsequent deposition of nanostructured multilayer Cr/(Cr-C)ml coating. The other novelty in the present study is related to the use of MF pulsed DC power supplies, operating at a fixed frequency of 100 kHz and a specific pulse shape, similar to the shape of HiPIMS pulses, for the deposition of nanostructured multilayer Cr/(Cr/a-C)ml coatings.