Iijima's observation in 1991 of fullerene-like materials by high-resolution transmission electron microscopy heralded the beginning of the carbon nanotube (CNT) era. A wealth of theoretical predictions and experimental verifications about CNTs have disclosed remarkable size- and structure-dependent properties that are attractive for various potential applications, ranging from conducting wires in molecular devices to fillers in nanocomposites. Many of these applications require assembly (alignment and/or patterning) of CNTs into hierarchical arrays over large-scale areas with controllable shape, location, orientation, and density of the nanotubes. Efforts from both the scientific and engineering points of view have been made to address this issue, beginning shortly after the discovery of CNTs. We review here the development of CNT-assembly techniques under the two rubrics of synthetic assembly and post-synthetic assembly, with emphasis given to the post-synthetic approach. Preliminary to the survey of assembly techniques, we also discuss the characterization techniques that have been widely used for the challenging tasks of visualizing and quantifying CNT assembly.