A series of isostructural noncatenated, water-stable zinc-based dipyridyl pillared-paddlewheel metal鈥搊rganic frameworks (MOFs) was synthesized with tunable pore hydrophobicity. Pore hydrophobicity was engendered through dipyridyl ligands decorated with alkyl chains of varying length (methyl to hexyl). The most hydrophobic MOFs exhibited selective sorption of ethanol over water.