Coffee ground waste from the coffee beverage preparation is mainly discarded and consequently ends up in landfill, which cause the contamination of caffeine in various environmental compartments. This study focuses on the upcycling of coffee-ground waste to carbon quantum dots (CQDs) for use as a modifying material to improve the visible light activity of titanium dioxide (TiO2). The CQD solution was synthesized by hydrothermal method, which has an average size of 2.80 ± 0.63 nm. The CQDs/TiO2 photocatalysts were prepared by combining CQD solutions at various amounts with sol-gel TiO2 and then coated on the fiberglass cloths (FGCs). The photocatalytic application mainly focuses on the removal of caffeine from the water. The photocatalytic experiment was preliminary run in a simple batch reactor under visible light. The 5CQDs/TiO2 coated FGC (5 mL of CQD solution/g of Ti-based on sol-gel) showed the best performance, and it was selected for the removal of caffeine and other pharmaceuticals (i.e., carbamazepine and ibuprofen) in the recirculating reactor. The removals of caffeine, carbamazepine, and ibuprofen after irradiation for 9 h were 82%, 88%, and 84%, respectively. The residual concentrations were significantly lower than the reported toxicity levels based on specific species. The changes in total organic carbon were observed, indicating the mineralization of pharmaceuticals in water. The 5CQDs/TiO2 coated FGC showed good flexible performance. No obvious loss of activity was observed for five runs. The actual wastewater from the coffee pot cleaning process was also tested. The removal was 80% for caffeine and 86% for color in the unit of the American Dye Manufacturers Institute (ADMI).