As shown in Fig. , water-surface interactions of ten distinct polymer surfaces are considered: seven based on amorphous polymers (PTFE, PE, PVC, PMMA, N66, PVA, and PVA † ) and three based on crystalline polymers (PE * , PVC * , and N66 * ). These polymers are both technologically important and chemically distinct (e.g., PE and PTFE are well , and N66 * . Amorphous surfaces formed by atactic and isotactic PVA (referenced as PVA † ) are also compared. Molecular images are visualized using OVITO. The elements are colored such that carbon is gray, fluorine is blue, chlorine is green, oxygen is red, and hydrogen is white; water molecules are cyan. known hydrophobic polymers with similar structure but the latter possesses fluorine; PVA, PMMA, and N66 have polar functional groups with the capacity for hydrogen-bonding; PVC possesses a chlorine that can attract water). Consequently, qualitatively different wetting behavior is expected across this set. A basic simulation setup consists of water (initially a droplet comprised of a specific number of water molecules) deposited atop a polymer configured into a slab geometry (Fig. ); three independent slabs are prepared to account for inhomogeneities and assess statistical convergence of behavior for amorphous polymer surfaces. The hydrophobicity of polymer surfaces is quantified using three metrics: a simulated nanoscale contact angle θ sim (larger is more hydrophobic, or for cos θ sim , more positive is more hydrophilic), a volume-adjusted excess chemical potential of water β μex w (N w ) (more positive is more hydrophobic), and a dehydration free energy β∆f σ (more positive is more hydrophilic). The sensitivity of some of the hydrophobicity metrics is probed by comparing behavior as the number of water molecules is changed (N = 2000, 1000, 500, 250, or 125 water molecules). The combination of different polymers, structural/stereochemical considerations, and droplet sizes yields (7 × 3 + 3) × 5 = 120 water-polymer surface systems for study.