AbstractThe contamination of soil and water by heavy metals poses a significant environmental and public health concern worldwide. To address this issue, a novel graphene quantum dot (GQD)‐based surface plasmon resonance (SPR) sensor is developed for the detection of mercury ions (Hg2+), a notorious heavy metal pollutant. The thiol and amine‐functionalized GQDs (S,N‐GQDs), synthesized via pyrolysis of citric acid and L‐cysteine, are directly immobilized onto the SPR chip surface without prior pretreatment, demonstrating their potential as efficient sensing materials. The SPR sensor exhibits high sensitivity and selectivity toward Hg2+ ions, as confirmed by kinetic binding analysis and isotherm modeling. The Langmuir isotherm model, which accurately describes the interactions between Hg2+ and S,N‐GQDs, provides insights into the sensor's mechanism of action. Furthermore, the sensor demonstrates robustness and reusability, with recoveries ranging from 98% to 104% over multiple cycles of analysis. Given the presence of contaminants in tap water, the developed sensor system holds significant importance for environmental monitoring and public health protection, offering a rapid, accurate, and cost‐effective solution for detecting Hg2+ ions in such samples. Overall, this study represents a significant advancement in the field of heavy metal detection, with potential implications for addressing environmental pollution and ensuring water quality.