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Carbon nanotubes (CNTs) of different alignments, such as surface-bounded and vertically aligned arrays, enable applications in different fields. In this study, controlled growth of CNTs with different alignments was achieved by electrically biasing catalyzed electrodes with different polarities in a laser-assisted chemical vapor deposition process. CNT growth was suggested to be guided by the movement of electrically charged catalyst-nanoparticles under the influence of an external electric field. This discovery provides a convenient approach to control the alignment of CNT arrays for different applications.