The physicochemical and mechanical properties of thin and freestanding heavy boron-doped diamond (BDD) nanosheets coated with a thin C:H:N:O plasma polymer were studied. First, diamond nanosheets were grown and doped with boron on a Ta substrate using the microwave plasma-enhanced chemical vapor deposition technique (MPECVD). Next, the BDD/Ta samples were covered with nylon 6.6 to improve their stability in harsh environments and flexibility during elastic deformations. Plasma polymer films with a thickness of the 500-1000 nm were obtained by magnetron sputtering of a bulk target of nylon 6.6. Hydrophilic nitrogen-rich C:H:N:O was prepared by the sputtering of nylon 6.6. C:H:N:O as a film with high surface energy improves adhesion in ambient conditions. The nylon-diamond interface was perfectly formed, and hence, the adhesion behavior could be attributed to the dissipation of viscoelastic energy originating from irreversible energy loss in soft polymer structure. Diamond surface heterogeneities have been shown to pin the contact edge, indicating that the retraction process causes instantaneous fluctuations on the surface in specified microscale regions. The observed Raman bands at 390, 275, and 220 cm −1 were weak; therefore, the obtained films exhibited a low level of nylon 6 polymerization and short-distance arrangement, indicating crystal symmetry and interchain interactions. The mechanical properties of the nylon-on-diamond were determined by a nanoindentation test in multiload mode. Increasing the maximum load during the nanoindentation test resulted in a decreased hardness of the fabricated structure. The integration of freestanding diamond nanosheets will make it possible to design flexible chemical multielectrode sensors.Materials 2020, 13, 1861 2 of 15 counterparts [4,5]. Since the first exfoliated graphene flake, the field of thin-layered materials and their possible applications have increased significantly, resulting in numerous papers on semiconducting nanomaterials including phosphorene [6], germanene [7], silicene [8], and carbon materials such as graphene [9], nanowall [10], and nanodiamond [11]. Nevertheless, the incorporation of nanoscale materials into various, well-defined architectures is still challenging. The majority of nanomaterials are fabricated with the requirement of a supporting substrate [12], which creates many obstacles in their integration into nanomaterial-based devices [13]. The design of these nanoscale devices demands the development of flexible freestanding nanostructures, providing additional accessibility to multidimensional interactions.Diamond, among other carbon materials, is recognized for its excellent mechanical [14] and optical [15] properties, and outstanding biocompatibility [16]. Even though pristine diamond is electrically insulating, it can become a semiconductor by incorporating dopants into its structure [17]. One of the most commonly used dopants is boron, changing diamond into a p-type semiconductor, and allowing diamond-based structures to be an important ...