The spatial arrangement of plasmonic nanoparticles can dramatically affect their interaction with electromagnetic waves, which offers an effective approach to systematically control their optical properties and manifest new phenomena. To this end, significant efforts were made to develop methodologies by which the assembly structure of metal nanoparticles can be controlled with high precision. Herein, recent advances in bottom-up chemical strategies toward the well-controlled assembly of plasmonic nanoparticles, including multicomponent and multifunctional systems are reviewed. Further, it is discussed how the progress in this area has paved the way toward the construction of smart dynamic nanostructures capable of on-demand, reversible structural changes that alter their properties in a predictable and reproducible manner. Finally, this review provides insight into the challenges, future directions, and perspectives in the field of controlled plasmonic assemblies.