The irrational usage of chemical substances including pesticides and drugs in agricultural and food production is a significant food safety issue due to its residues. Therefore, the detection of harmful residues in foods is an indispensable step for guaranteeing the consumer's health. Conventional methods, such as HPLC, GC-MS and LC-MS are accurate enough, but they fail to meet the requirements of the modern industry for rapid and on-line detection. Novel reliable techniques should thus be developed as alternatives. In this review, fundamentals of surface-enhanced Raman spectroscopy (SERS) is introduced. Recent advances in its usage for detecting harmful chemical residues in agricultural products including pesticides, antibiotics and β2-adrenergic agonists are discussed by two typical ways of detection improvement, and the advantages of SERS are addressed. Finally, future trends to routine use of SERS applications in harmful residues are presented. SERS is a promising detection technique for the detection of common harmful chemical residues with merits of simple sampling, rapid data collection and non-destructiveness. Despite rapid developments in the technology, there is much studies should be done before SERS could be used as a daily tool for the industry. •Principles of surface-enhanced Raman spectroscopy (SERS) are introduced.•Recent applications of SERS for harmful residues detection are reported.•Future perspectives and limitations of SERS are discussed.•More studies should be done for possible daily use of SERS in the industry.