There is an increasing interest in recent years in using novel nanomaterials as cost-effective, sensitive, and reproducible substrate for surface-enhanced Raman spectroscopy (SERS) applications. In this study, a novel SERS substrate was developed by assembling gold nanorods into standing arrays on a gold-coated silicon slide. The standing nanorod arrays were closely packed on the gold film, generating strong electromagnetic field and uniformly distributed SERS "hot-spots" on the array surface. The as-prepared SERS substrates were used to detect a widely used pesticide (that is, carbaryl) in acetonitrile-water solution, apple juice, and cabbage. Results demonstrate that the actual concentrations of carbaryl in apple juice and cabbage were linearly correlated with the concentrations predicted by the multiple linear regression models (R > 0.97). The detection limits of carbaryl in apple juice and cabbage were both 2.5 ppm, meeting the maximum residue limits set by US Environmental Protection Agency (EPA). SERS can detect as low as 0.1 ppm of carbaryl in acetonitrile-water solution. In addition, satisfactory recoveries were obtained for carbaryl in both apple juice and cabbage. These results indicate that SERS coupled with the standing gold nanorod array substrates is a sensitive and reproducible method and can accurately detect pesticides in foods.