The concept of nanoparticles (NPs) as building blocks offers new possibilities to produce complex and tailored structures from the nano- to the mesoscale. In order to control a “polymerization” of particles, knowledge of the mechanism and kinetics of the reaction are necessary. We show that controlled assembly of cetylpyridinium chloride-stabilized gold NPs utilizing induced dipole–dipole interactions can lead to the formation of defined one-dimensional structures in solution. Three different shaped NPs (cubes, octahedra, and truncated cuboctahedra) were investigated individually. The assembly process is analogous to a step growth polymerization and is quantitatively describable with kinetics of a polyesterification. In situ kinetic studies reveal that there is an ideal particle size and shape for the induced dipole-driven assembly. Even small changes in size have remarkable effects on the assembly behavior. We further demonstrate that the transition from oriented assembly to oriented attachment requires a critical particle size (critical interface area) resulting from a size-dependent energy barrier for the crystallographic fusion. A combination of ideal size, shape, and degree of destabilization enables controlled oriented attachment of gold NPs in solution to chainlike structures under ambient conditions.