Surface-enhanced Raman spectroscopy (SERS) was used for rapid detection of sodium thiocyanate in milk employing silver aggregates as active substrate. Silver nanoparticles were induced to silver aggregates by trichloroacetic acid (TCA). The limit of detection (LOD) for sodium thiocyanate was 10−2 µg ml−1 in water with an analytical enhancement factor of 5.4 × 106. The silver aggregates represent good reproducibility and stability. Good linear relationship was obtained for sodium thiocyanate in milk at concentration ranges from 0.1 to 10 µg ml−1 (R2 = 0.995). Using TCA as protein precipitator, silver colloid would aggregate spontaneously when mixing with samples during SERS measurement without the need of additional aggregating agent. The simple pretreatment procedures and analytical methods are less time consuming (<10 min) and environmentally friendly, making the proposed method much practical for in situ detection of sodium thiocyanate in market milk. Copyright © 2014 John Wiley & Sons, Ltd.