The precise control over the locations of hot spots in a nanostructured ensemble is of great importance in plasmon-enhanced spectroscopy, chemical sensing, and super-resolution optical imaging. However, for multiparticle configurations over metal films that involve localized and propagating surface plasmon modes, the locations of hot spots are difficult to predict due to complex plasmon competition and synergistic effects. In this work, theoretical simulations based on multiparticle–film configurations predict that the locations of hot spots can be efficiently controlled in the particle–particle gaps, the particle–film junctions, or in both, by suppressing or promoting specific plasmonic coupling effects in specific wavelength ranges. These findings offer an avenue to obtain strong Raman signals from molecules situated on single crystal surfaces and simultaneously avoid signal interference from particle–particle gaps.