Environmentally resilient antimicrobial coatings are becoming increasingly required for a wide range of applications. For this purpose, nanocomposite thin films of poly(vinylidene fluoride) (PVDF) filled with several types of functionalized nanodiamonds (NDs) were processed by solvent casting. The effects of ND inclusion and functionalization in their morphological, structural, optical, thermal, and electrical properties were evaluated taking into account the type of the nanofiller and a concentration up to 2 wt %. The morphology, structure, and thermal features of the polymer matrix are governed by the processing conditions, and no noticeable changes occurred due to the presence of the ND fillers. The polymer crystallized mainly in the α phase with a crystallinity of ≈60%. In turn, the optical transmittance from 200 to 800 nm and the dielectric constant effectively depended on the ND type and content. The inclusion of the ND particles effectively provided antimicrobial properties to the films, which depended on the ND functionalization. This study thus shows that the incorporation of functionalized NDs into PVDF allows the development of antimicrobial coatings with tailorable optical and dielectric properties, which could be of great importance to face nowadays pandemic crisis scenario.