Coupling of localized surface plasmon resonances results in singular effects at the void space between noble metal nanoparticles. However, implementation of practical applications based on plasmon coupling calls for the high yield production of metal nanoparticle clusters (dimers, trimers, tetramers, …) with small gaps. Therefore, controlled assembly using colloid chemistry methods is an emerging and promising field. We present a brief overview over the controlled assembly of plasmonic nanoparticle clusters by colloid chemistry methods, together with a description of their plasmonic properties and some applications, with an emphasis in sensing through surface-enhanced Raman scattering spectroscopy for bio-detection purposes. We point out the important role of separation methods to obtain colloidal clusters in high yield. A special encouragement to explore assembly of anisotropic building blocks is pursued.