Open-air aerosol-assisted plasma deposition has emerged as an efficient process to deposit innovative composite coatings. In this work, it was used to investigate biodegradable polymeric coatings loaded with carbon dots (CDs) for bioengineering and biomedical applications. The structure, composition, wettability, and biodegradation of these coatings depend on the precursors used, here methacrylic anhydride and ethylene glycol di-methacrylate. The effectiveness of the deposition was confirmed by X-ray photoelectron and Fourier-transformed infrared spectroscopies, i.e., polymerization of vinyl groups and integrity of hydrolysable functions. The latter allow control the CDs release over time, which were homogenously distributed in the coating, as confirmed by electronic and confocal microscopies. Both coatings were found to be non-cytotoxic to human dermal fibroblasts. This one-step open-air acrylate-based plasma deposition strategy has enabled the tuning of the coating release profile and offers new perspectives for drug delivery applications.