The past a few years have witnessed the wide use of metallic nanoparticles as ideal reporters for colorimetric detection, which generally involves an analyte-triggered alteration of aggregation degree of applied nanoparticles, and thus the change of colloidal color. However, these aggregation-based colorimetric probe are associated with a number of drawbacks, including poor stability of nanoaggregates, requirement of complicated functionalization and non-linearity of output signals. To address these problems, we herein employ mesoporous silica-coated gold nanorods (MS AuNRs) as novel nanocomposites for non-aggregation-based label-free colorimetric sensing relying on their chemical redox-modulated surface chemistry. In our sensing system, Hg(2+) ions are reduced to Hg(0) depositing on the surface of MS AuNPs and result in a great color change of MS AuNRs, while the subsequent introduction of S(2-) leads to a reverse process owing to the extraction of Hg(0) by S(2-). The experimental results for colorimetric sensing of Hg(2+) and S(2-) imply considerable sensitivity and specificity, suggesting the high potential of our approach for rapid environmental monitoring and bioanalysis in the future.