摘要： Graphene quantum dots (GQDs) have been demonstrated of great potential and benefits in the fields of bioimaging and white light-emitting-diodes (WLEDs). However, it is still highly demanding at the current level to solve the dilemma of achieving high-yield GQDs of good quality and superior fluorescent property using low-cost sustainable and industrializable production procedure. In this work, we for the first time report the gram-scale synthesis of well-crystalline GQDs with ultra-small size based on thermal-driven Advanced Oxidation Process (AOP) under facile green hydrothermal conditions. The average yield calculated from 20 trials reached up to 60%, and the average size of the dots was measured to be ~3.7 nm. Furtherly, GQDs with the photoluminescence (PL) emission of blue, green, yellow, orange, and red have been prepared by expanding the π-conjugation and introducing graphite nitrogen in the carbon skeleton based on chemical structure engineering. The PL-tunable GQDs have an average size distribution of 2~5 nm and a lamellar structure of 2~6 layers. Structure analysis results have indicated that the red shift of PL emission is attributed to bandgap narrowing. This approach successfully converts the easily available and cheap precursor into high-valued products with great application potentials. The PL-tunable GQDs have been successfully used as fluorescent probes of good biocompatibility for in vitro/ in vivo bio-imaging and to produce highly-photostable white-light-emitting composite film with a quantum yield (QY) of 24%.