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The search for efficient amine-functionalized materials for direct air capture (DAC) of CO2 is highly important to achieve negative emissions. Here we report a new family of class 1 adsorbents for DAC by loading 67 wt% branched poly(ethylenimine) (PEI) onto Mg–Al–CO3 layered double hydroxide-derived mixed metal oxides (MMOs), which exhibit unexpectedly large CO2 uptakes (2.27 mmol g−1), fast kinetics (1.1 mmol g−1 h−1), and high stability over 20 cycles at 25 °C under 0.4 mbar CO2. The prepared MMO nanosheets are self-assembled into spherical shaped particles with abundant slit-like mesopores and broad pore size distribution. This ideal nanostructure leads to the uniform distribution of the impregnated PEIs and optimal accessibility for CO2 molecules. The defect-abundant MMO layers provide strong electrostatic attraction to the attached polyamines, making the hybrid adsorbents thermally robust up …