In this paper, the surface properties and selected mechanical and biological properties of various multi-layer systems based on diamond-like carbon structure deposited on low-density polyethylene (LDPE) substrate were studied. Plasma etching and layers deposition (incl. DLC, N-DLC, Si-DLC) were carried out using the RF CVD (radio frequency chemical vapor deposition) method. In particular, polyethylene with deposited N-DLC and DLC layers in one process was characterized by a surface hardness ca. seven times (up to ca. 2.3 GPa) higher than the unmodified substrate. Additionally, its surface roughness was determined to be almost two times higher than the respective plasma-untreated polymer. It is noteworthy that plasma-modified LDPE showed no significant cytotoxicity in vitro. Thus, based on the current research results, it is concluded that a multilayer system (based on DLC coatings) obtained using plasma treatment of the LDPE surface can be proposed as a prospective solution for improving mechanical properties while maintaining biocompatibility.