Materials science has observed a continuous increase in the use of metal nanoparticles in a wide range of studies, from fundamental physics to technological applications such as photocatalysis and optical communication devices. This broad scope has the same fundamental origin, the localized surface plasmons, whose excitation leads to strong light confinement, especially in the vicinity of closely spaced nanoparticles, the hot spots. The field amplification may be used to amplify the Raman scattering of adsorbed molecules, which is known as surface-enhanced Raman scattering (SERS). A crucial and limiting characteristic of SERS hot spots is their very localized nature, that influences the SERS intensity reproducibility as well as the probabilities of observation of single-molecule SERS signals. In this paper we discuss the correlation between SERS performance and gold nanorod cluster structures using transmission electron microscopy, SERS spectra and numerical simulations. The experimental data showed interesting behavior for the combination of end-to-end and side-by-side interactions, revealing the possibility of creating strong hot spots with a more extended spatial distribution. The results give insights into the development of high-performance SERS substrates.