Abstract Carbon nanotube fibers (CNTFs) are endowed with excellent mechanical, electrical, and thermal properties and are considered promising candidates in numerous cutting‐edge fields. However, the inherent black color of CNTFs hinders their practical application in fields with high aesthetic requirements such as wearable devices and smart textiles. Due to the smooth surface and chemical inertness, CNTFs are hard to be dyed by conventional chemical dyes or colorful inks. Herein, we realize a structural coloration of CNTFs by coating them with two metal oxide layers via atomic layer deposition. The three elements of color, that is, hue, saturation, and brightness, can be controlled by adjusting the types and thickness of each oxide layer. Colorful CNTFs with wide color gamut and high saturation are achieved through different combinations. A film interference model is also established to reveal the mechanism of the structural coloration, which is a comprehensive result of thin‐film interference and surface roughness briefly. The calculated reflectance well fits the measured results by introducing surface roughness parameters. Moreover, the colored CNTFs are not iridescent because of retinal signal delay, which will further expand their applications.
