Graphene quantum dots (GQDs) are attractive materials for use as highly selective and sensitive chemical sensors, owing to their simple preparation and affordability. GQDs have been successfully deployed as sensors for toxic metal ions, which is a significant issue due to the ever-increasing environmental contamination from agricultural and industrial activities. Despite the success of GQDs in this area, the mechanisms which underpin GQD-metal ion specificity are rarely explored. This lack of information can result in difficulties when attempting to replicate published procedures and can limit the judicious design of new highly selective GQD sensors. Furthermore, there is a dearth of GQD examples which selectively detect biologically relevant alkali and alkaline earth metals. This review will present the current state of GQDs as metal ion sensors for harmful contaminants, highlighting and discussing the discrepancies that exist in the proposed mechanisms regarding metal ion selectivity. The emerging field of GQD sensors for biorelevant metal ion species will also be reviewed, with a perspective to the future of this highly versatile material.