Graphene quantum dots (GQDs) have drawn tremendous attention on account of their numerous alluring properties and a wide range of application potentials. Here, we report that hydrophilic and hydrophobic N-doped GQDs can be prepared via exfoliating and disintegrating graphite flakes. Various spectroscopic characterizations including TEM, AFM, FTIR, PL, XPS, and Raman spectroscopy demonstrated that the hydrophilic N-doped GQDs (IN-GQDs) and the hydrophobic N-doped GQDs (ON-GQDs) are mono-layered and multi-layered, respectively. In terms of practical aspects, the supercapacitor of an ON-GQDs/SWCNTs composite paper electrode was fabricated and exhibited an areal capacitance of 114 mF/cm2, which is more than 250% higher than the best reported value to date for a GQDs/carbon nanotube hybrid composite. For IN-GQDs applications, bio-memristor devices of IN-GQDs-albumen combination exhibited on/off current ratios in excess of 104 accompanied by stable switching endurance of over 250 cycles. The resistance stability of the high resistance state and the low resistance state could be maintained for over 104 s. Moreover, the IN-GQDs exhibited a superior quantum yield (34%), excellent stability of cellular imaging, and no cytotoxicity. Hence, the solution-based method for synchronized production of IN-GQDs and ON-GQDs is a facile and processable route that will bring GQDs-based electronics and composites closer to actualization.