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Physisorbent metal–organic materials (MOMs) have shown benchmark performance for highly selective CO₂ capture from bulk and trace gas mixtures. However, gas stream moisture can be detrimental to both adsorbent performance and hydrolytic stability. One of the most effective methods to solve this issue is to transform the adsorbent surface from hydrophilic to hydrophobic. Herein, we present a facile approach for coating MOMs with organic polymers to afford improved hydrophobicity and hydrolytic stability under humid conditions. The impact of gas stream moisture on CO₂ capture for the composite materials was found to be negligible under both bulk and trace CO₂ capture conditions with significant improvements in regeneration times and energy requirements.