Dopamine (DA) is a neurotransmitter which plays a key role in the life science. Self-assembled [email protected] nanorod dimers based on aptamers were developed for ultrasensitive dopamine detection. The electronic field was significantly enhanced by the addition of silver shell coating on the surface of Au NR dimer. The results displayed that [email protected] NR dimers were ideal building blocks for constructing the SERS substrates with prominent Raman enhancement effects. It was found that with using this Surface-enhanced Raman scattering (SERS)-encoded this sensing system, a limit of detection of 0.006 pM and a wide linear range of 0.01–10 pM for dopamine detection were obtained. Our work open up a new avenue for the diagnosis and drug-discovery programs.