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The design of high-efficiency CO₂ adsorbents with low cost, high capacity, and easy desorption is of high significance for reducing carbon emissions, which yet remains a great challenge. This work proposes a facile construction strategy of amino-functional dynamic covalent materials for effective CO₂ capture from flue gas. Upon the dynamic imine assembly of N-site rich motif and aldehyde-based spacers, nanospheres and hollow nanotubes with spongy pores were constructed spontaneously at room temperature. A commercial amino-functional molecule tetraethylenepentamine could be facilely introduced into the dynamic covalent materials by virtue of the dynamic nature of imine assembly, thus inducing a high CO₂ capacity (1.27 mmol·g⁻¹) from simulated flue gas at 75 °C. This dynamic imine assembly strategy endowed the dynamic covalent materials with facile preparation, low cost, excellent CO₂ capacity, and outstanding cyclic stability, providing a mild and controllable approach for the development of competitive CO₂ adsorbents.