  Because of their natural one-dimensional (1D) structure combined with
intricate chiral variations, carbon nanotubes (CNTs) exhibit various
exceptional physical properties, such as ultrahigh electrical and thermal
conductivity, exceptional mechanical strength, and chirality-dependent
metallicity. These properties make CNTs highly promising for diverse
applications, including field-effect transistors, sensors, photodetectors, and
thermoelectric devices. While CNTs excel individually at the nanoscale, their
1D and chiral nature can be lost on a macroscopic scale when they are randomly
assembled. Therefore, the alignment and organization of CNTs in macroscopic
structures is crucial for harnessing their full potential. In this review, we
explore recent advancements in understanding CNT alignment mechanisms,
improving CNT aligning methods, and demonstrating macroscopically 1D properties
of ordered CNT assemblies. We also focus on a newly discovered class of CNT
architectures, combining CNT alignment and twisting mechanisms to create
artificial radial and chiral CNT films at wafer scales. Finally, we summarize
recent developments related to aligned and chiral CNT films in optoelectronics,
highlighting their unique roles in solar cells, thermal emitters, and optical
modulators.
