A facile dry route electrostatic-force-directed assembly (ESFDA) was used to deposit silver nanocrystalsonto the external surface of vertically aligned multiwalled carbon nanotubes (MWCNTs). Charged andnonagglomerated aerosol silver nanocrystals were first produced using a mini-arc plasma source. Thenanocrystals were then assembled onto the electrically biased MWCNT array through the enhanced electricfield near the CNT surface. The electrostatic field plays a crucial role in the assembly process. Gradients ofthe nanocrystal size and the nanocrystal areal density along the length of the CNT have been observed, andthese are likely due to the variation of the electric field near the CNT surface. The ESFDA technique enablesthe in situ coating of CNT arrays with nanocrystals to create novel hybrid nanomaterials with tailored properties.