Nanoscale morphology of vanadium dioxide (VO2) films can be controlled to realize smooth ultrathin (<10 nm) crystalline films or nanoparticles with atomic layer deposition, opening doors to practical VO2 metal-insulator transition (MIT) nanoelectronics. The precursor combination, the valence of V, and the density for as-deposited VO2 films, as well as the postdeposition crystallization annealing conditions determine whether a continuous thin film or nanoparticle morphology is obtained. It is demonstrated that the films and particles possess both a structural and an electronic transition. The resistivity of ultrathin films changes by more than two orders of magnitude across the MIT, demonstrating their high quality.