A novel concept is proposed for converting, liquid-phase colorimetric assay into enhanced surface-tethered electrochemical analysis, which is based on the analyte-induced formation of a network architecture of metal narioparticles (MNs). In a proof-of-concept trial, thymine-functionalized silver nanoparticle (Ag-T) is designed as the sensing unit for Hg2+ determination. Through a specific T-Hg2+-T coordination, the validation system based on functionalized sensing units not only can perform well in a colorimetric Hg2+ assay, but also can be developed into a more sensitive and stable electrochemical Hg2+ sensor. In electrochemical analysis, the simple principle Of analyte-induced aggregation Of MNs can be used as a dual signal amplification strategy for significantly improving the detection sensitivity. More importantly, those numerous and diverse colorimetric assays that rely on the target-induced aggregation of MNs an be augmented to satisfy the ambitious demands of sensitive analysis by converting them into electrochemical assays via this approach.