A facile approach for adding moisture resistance to transparent nematic aerogels composed of individualized cellulose nanofibers (i-CNF) at full preservation of the anisotropic aerogel structure is presented. Sequential nitroxide-mediated oxidation and mechanical cellulose fiber delamination were applied to obtain i-CNF dispersions in water. Nematic ordering caused by repulsive forces between i-CNF surface carboxylate groups was set by acid-induced hydrogen bonding and gelation, respectively. Solvent exchange to acetone, impregnation with the PMMA, scCO 2 -mediated antisolvent precipitation of the secondary polymer, and scCO 2 extraction of interstitial acetone afforded highly hydrophobic nanocomposite aerogels. Birefringence studies utilizing polarized light and the Michel−Levy Chart to evaluate interference patterns revealed that nematic i-CNF ordering is virtually not affected by the respective surface modification and scCO 2 drying steps. Morphological studies provide evidence that the large internal surface (>500 m 2 g −1 ) of the hybrid aerogels consists of a homogeneous ultrathin PMMA (mono)layer that virtually does not affect the high porosity (≥99%) and transparency (>77% transmission, 600 nm, 2.13 mm thickness) inherent to i-CNF aerogels. The obtained materials exhibited excellent resistance toward moisture as apparent from the high water contact angle (119.4°± 7.5). As PMMA imparts the aerogel stiffness and hydrophobicity, aggregation of nanofibrils in moist environment or under vacuum conditions can be avoided even at ultralow densities as low as 9.6 mg cm −3 .