A simple colorimetric assay with high sensitivity, excellent selectivity and a tunable dynamic range is reported for detecting trace amounts of mercuric ion in aqueous solution based on the coordination of Hg2+ to the gold nanoparticle (AuNP)-associated 3-nitro-1H-1,2,4-triazole (NTA). The NTA can stabilize the AuNPs against tris-induced aggregation through capping the AuNPs. In the presence of Hg2+, the NTA is released from the AuNP surface via the formation of a NTA-Hg2+ coordination complex, leading to the aggregation of AuNPs in tris. This detection strategy is unique in terms of high sensitivity and excellent selectivity, a tunable dynamic range, and simplicity of probe preparation. Low detection limits of 7 nM (1.4 ppb) and 50 nM (10 ppb) can be achieved by spectrophotometer and by direct visualization, respectively, under the optimized conditions. No noticeable colour changes are observed towards other metal ions (Ag+, Zn2+, Ni2+, Cr3+, Mg2+, Cu2+, Co2+, Cd2+, Pb2+, Fe2+) at concentrations up to 100 μM without the need of any other masking agents. In addition, the dynamic range of the assay can be easily tuned by adjusting the amount of NTA in the NTA-AuNP probes. More importantly, the NTA-AuNP probes can be simply prepared by mixing NTA with as-synthesized citrate-capped AuNPs. This not only avoids complicated surface modifications and tedious separation processes, but also is cost-effective.