Dielectrophoresis drives the motion of nanoparticles through the interaction of their induced dipoles with a non-uniform electric field. We experimentally observe rf dielectrophoresis on 100 nm diameter gold nanoparticles in a solution and show that for MHz frequencies, the nanoparticles can reversibly aggregate at electrode gaps. A frequency resonance is observed at which reversible trapping of gold nanoparticle “clouds” occurs in the gap center, producing almost a 1000-fold increase in density. Through accounting for gold cores surrounded by a conducting double layer ion shell, a simple model accounts for this reversibility. This suggests that substantial control over nanoparticle separation is possible, enabling the formation of equilibrium nanoarchitectures in specific locations.