This paper proposes a selective strategy for quantitative detecting cardiac troponin I (cTnI) in clinical serum samples by using Raman spectroscopy combined with magnetic molecularly imprinted polymers (MMIPs). The signature peptide was selected as a template for molecular imprinting due to its chemical stability and small molecular mass. MMIPs were synthetized with the signature peptide as template and methylacrylic acid as monomer in presence of vinyl-modified magnetic particles. MMIPs with high magnetic character and adsorption properties were able to be stained by Coomassie Brilliant Blue G-250 after the target template was specifically captured, which showing a characteristic absorption peak at Raman shift 1610 cm−1. The Raman signal intensity at 1610 cm−1 showed a linear relationship in the 0.01 to 100 ng·mL−1 concentration range. The recovery of cTnI in serum were 92.7–111.2 % with relative standard deviation in the range of 2.51 % to 8.52 %. This paper has important practical application for preliminary rapid detection of cTnI in clinical serum samples.