Broadband‐Responsive UiO‐PPy MOF Micromotors for 3D Motion and Selective Dye Separation

ABSTRACT Light‐driven micro/nanomotors (MNMs) have emerged as promising candidates for environmental remediation and related applications. However, conventional light‐driven systems often suffer from poor light‐harvesting efficiency, limited motion modes, and high fabrication costs, which hinder their practical employment. Herein, we developed a novel class of MNMs capable of efficient propulsion across a broad UV–Vis–NIR spectral range. These hybrid motors are based on the robust metal–organic framework UiO─66 and functionalized with polypyrrole (PPy) through three distinct integration strategies: in situ polymerization, pre‐loading, and post‐synthetic modification. The resulting MNMs enable tunable motion behaviors and catalytic performance. Among them, UiO‐PPy‐PreInc motors exhibited outstanding photothermal response and achieved ultrafast propulsion speeds up to 1717 ± 265 µm/s under UV light irradiation. Comprehensive trajectory analyses revealed dynamic 3D motion, including directional steering and adaptive velocity control. A custom‐built optical microscopy tracking system enabled real‐time, high‐resolution monitoring of their behavior, which was previously achievable only through computational simulations. Furthermore, the synergistic combination of UiO─66's high surface area and porosity with PPy's photothermal and charge transport properties facilitated highly efficient methyl orange degradation (99%) and selective dye separation (90%) under light activation. This work establishes a versatile and scalable platform for multifunctional MNMs with integrated pollutant removal and resource recovery capabilities, paving the way toward advanced water purification technologies.