Atomic-scale material deposition is utilized to achieve uniform coverage and modification of the surface properties of natural fiber and woven fabric materials, where irregular nanoscale features are embedded in a macroscale interpenetrating fiber network. The complex surface topology of the woven fabric results in significantly different film-growth thickness per ALD cycle as compared to planar surfaces coated using the same process conditions, likely due to reactant adsorption within the fiber starting material, as well as impeded reactant transport out of the fabric system during the purge cycle. Cotton textiles modified with conformal nanoscale Al2O3 are found to show extreme hydrophobic effects, distinctly different from planar surfaces that receive the same coatings. The results highlight key concerns for achieving controlled conformal coatings on complex surfaces and open the possibility for new textile finishing approaches to create novel fabric-based materials with specialized function and performance.