Carbon dots (CDs), owing to their excellent photoluminescent features, have been extensively studied for physics preparation methods and for biomedical and optoelectronic device applications. The assessment of the applicability of CDs in the production of luminescent polymeric composites used in LEDs, displays, sensors, and wearable devices is being pursued. The present study reports on an original, environmentally friendly, and low-cost route for the production of carbon dots with an average size of 4 nm by laser ablation in liquid. Jointly, to prove the significance of the study for a wide range of applications, a free-standing flexible polyvinyl alcohol (PVA) composite containing photoluminescent carbon dots was manufactured. CDs were prepared using targets of porose charcoal with a density of 0.271 g/cm3 placed in phosphate-buffered saline (PBS) liquid solution and irradiated for 30 min by pulsed IR diode laser. The optical properties of the obtained suspension containing carbon dots were studied with UV-ViS and FTIR spectroscopies. The photoluminescence of the produced carbon dots was confirmed by the emission peak at 480 nm in the luminescence spectrum. A narrow luminescence band with a full width at half-maximum (FWHM) of less than 40 nm could be an asset in spectral emission analysis in different applications. Atomic force microscopy confirms the feasibility of manufacturing CDs in clean and biocompatible environments, paving the way for an easier and faster production route, crucial for their wider applicability.