Single‐Stimulus‐Induced Modulation of Multiple Optical Properties

Stimuli‐responsive smart optical materials hold great promise for applications in active optics, display, sensing, energy conversion, military camouflage, and artificial intelligence. However, their applications are greatly restricted by the difficulty of tuning different optical properties within the same material, especially by a single stimulus. Here, magnetic modulations of multiple optical properties are demonstrated in a crystalline colloidal array (CCA) of magnetic nanorods. Small‐angle X‐ray scattering studies reveal that these nanorods form an unusual monoclinic crystal in concentrated suspensions. The CCA exhibits optical anisotropy in the form of a photonic bandgap and birefringence, thus enabling magnetic tuning of the structural color and transmittance at a rate of 50 Hz. As a proof‐of‐concept, it is further demonstrated that the fabrication of a multifunctional device for display, anticounterfeiting, and smart‐window applications based on this multiple magneto‐optical effect. The study not only provides a new model system for understanding colloidal assembly, but also opens up opportunities for new applications of smart optical materials for various purposes. A new type of smart optical material based on the nanorod crystalline colloidal array (CCA) is developed, which enables the modulation of two optical properties by the same stimulus. An unusual monoclinic crystal structure is formed in the CCA. This work will provide a new smart optical platform with interesting implications for a variety of purposes.