Exosomal miRNA expression derived from tumor cells provides a valuable and promising noninvasive modality for the early diagnosis and assessment of the efficacy of cancer treatment. However, accurate detection and identification of miRNA within exosomes have been challenging due to its low abundance and the complexity and tedious extraction with large sample volumes in the separation process. Here, we developed an electrically activated nanoplatform for rapid and sensitive detection and identification of exosome miRNA, through triggering miRNA release by opening exosomes that were captured on the electrode surface using a slightly applied electric field (50 mV), and simultaneously detected them with surface-enhanced Raman spectroscopy (SERS) in situ. The method possessed superior specificity and sensitivity for exosomal miRNA detection, with a low detection concentration of 0.5 nM. The SERS sensor chips also showed a superior sensing performance of exosomal miRNA in complex body fluids such as urine and blood. We found that exosomal miRNA contents derived from tumor cells were significantly higher than those in normal cells, and importantly, the concentrations of exosomes secreted from three different cell lines were distinctly augmented after mild electrical stimulation (ES) treatment. Furthermore, the miRNA expression within exosomes was upregulated after the ES treatment of cells. The developed approach and SERS detection platform for exosomal miRNA are promising for noninvasive and precise screening, classification, and monitoring of cancer.