Assemblies of plasmonic nanoparticles enable new modalities for biosensing. Engineered superstructures from metal nanoparticles can enhance the plasmon resonances and chiroptical activity of nanoscale dispersions. Such phenomena are keys to the fabrication of highly sensitive, selective and fast-responding detection platforms, making them promising candidates for clinical applications. This tutorial review summarizes and discusses recent advances in this area. The topics covered in the review include the basic strategies adopted for assembly and engineering of plasmonic nanoparticles, optical properties of the assembled nanostructures and their applications to both in vitro and in vivo detection of biological compounds. We also offer our vision of the future prospects of this field of research. Among emerging applications in this area are novel nanosensors and platforms, for food safety, environmental monitoring, health safeguarding, as well as biodefense.