An electrohydrodynamic methodology has been developed that makes possible the precise assembly of two- and three-dimensional colloidal crystals on electrode surfaces. Electrophoretically deposited colloidal particles were observed to move toward one another over very large distances (greater than five particle diameters) to form two-dimensional colloidal crystals for both micrometer- and nanometer-size particles, This coalescence of particles with the same charge is opposite to what is expected from electrostatic considerations and appears to result from electrohydrodynamic fluid flow arising from an ionic current flowing through the solution. The ability to modulate this ''lateral attraction'' between particles, by adjusting field strength or frequency, facilitates the reversible formation of two-dimensional fluid and crystalline colloidal states on the electrode surface. Further manipulation allows controlled structures to be assembled.