In this study, the silicon-based interlayers for hydrogenated amorphous carbon (a-C:H) coating on a chromium-plated substrate are presented. The a-Si, a-Si:N, a-Si:H and a-SixCy:H interlayers with a thickness of about 306 nm were deposited by direct current magnetron sputtering technique. The a-C:H films with a thickness of about 317 nm was prepared as a top layer by radio frequency-plasma chemical vapor deposition. The a-C:H films with silicon-based interlayers were characterized by x-ray photoelectron spectroscopy, Raman spectroscopy, field emission-secondary electron microscopy, nanoindentation, micro-scratching, and electrochemical corrosion measurements in terms of their structure, morphology, mechanical and adhesive properties, and corrosion resistance. The a-C:H films with an a-Si:H interlayer exhibit the lowest corrosion current density, which is about 36 times lower than that of the uncoated chromium-plated substrate. In addition, the hardness increases from 8.48 GPa for the uncoated substrate to 20.98 GPa for the a-C:H/a-Si:H sample. The mixing with hydrogen gas could reduce the residual oxygen during the deposition process, which could reduce the Si–O bonding and improve the adhesion strength between the a-C:H film and the a-Si:H interlayer and the a-Si:H interlayer and the substrate. Therefore, it can be concluded that the protective a-C:H coating with an a-Si:H interlayer has excellent potential to significantly improve the durability and extend the service life of materials used in abrasive and corrosive environments.