Controllable and selective synthesis is essential for many potential applications of gold nanocrystals in nanodevice manufacturing. In the current article, a hybrid technology that integrates electrodeposition with dielectrophoresis is reported, demonstrating the controllable fabrication of nanostructures with desirable dimensionality and morphology, such as particles, aligned nanowires, networks, coral-like morphologies, and three-dimensional branched nanocrystals on a scaffold. The current experiments and calculations reveal the dependence of morphology on electrode geometry and electric field parameters. The proposed templateless and facile technology offers great potential for the rational synthesis of other metallic nanomaterials with controllable morphology for advanced functional applications. (C) 2011 The Electrochemical Society. [DOI: 10.1149/2.017202esl] All rights reserved.