The expression of microRNAs (miRNAs) is critical in gene regulation and has been counted into disease diagnosis marks. Precise imaging and quantification of miRNAs could afford the important information for clinical diagnosis. Here, two smart binary star ratio (BSR) probes were designed and constructed, and miRNA triggered the connection of the binary star probes and the reciprocal changes of dual signals in living cells. This multifunctional probe integrates fluorescence and surface enhanced Raman scattering (SERS) imaging, with enzyme-free numerator signal amplification for dual-mode imaging and dual-signal quantitative analysis of miRNA. First, compared with the single-mode ratio imaging method, using fluorescence-SERS complementary ratio imaging, this probe enables more accurate imaging contrast for direct visualization signal changes in living cells. Multiscale information about the dynamic behavior of miRNA and the probe is acquired. Next, via SERS reverse signal ratio response and a novel enzyme-free numerator signal amplification, the amplified signal and reduced black value were achieved in the quantification of miRNA. More importantly, BSR probes showed good stability in cells and were successfully used for accurate tracing and quantification of miR-203 from MCF-7 cells. Therefore, the reported BSR probe is a potential tool for the reliable monitoring of biomolecule dynamics in living cells.