Anisotropic metallic nanoparticles (NPs) have unique optical properties, which lend them to applications such as surface-enhanced Raman scattering (SERS) spectroscopy. Star-shaped gold (Au) NPs were prepared in aqueous solutions by the seed-mediated growth method and tested for Raman enhancement using 2-mercaptopyridine (2-MPy) and crystal violet (CV) probing molecules. For both molecules, the SERS activity of the nanostars was notably stronger than that of the spherical Au NPs of similar size. The Raman enhancement factors (EFs) for 2-MPy on Au nanostars and nanorods are comparable and estimated as greater than 5 orders of magnitude. However, the enhancement for CV on nanostars was significantly higher than for nanorods, in particular at CV concentrations of 100 nm or lower. This article is a US Government work and is in the public domain in the USA. Published in 2008 by John Wiley & Sons, Ltd.