Surface‐Selective Nucleation of Polymeric Resists for Bottom‐Up Nanofabrication

Bottom‐up micro/nanofabrication complements photolithography in multilayer, 3D, and cost‐effective manufacturing, but lacks resist patterning technology with photoresist‐level reproducibility, processability, and universality. Here, we explore a surface‐selective nucleation (SSN) effect to derive polymeric resist patterns with nanoscale resolution, inherent 3D compatibility, low defect density, clean lift‐off, and broad applicability across fabrication platforms. The SSN phenomenon is achieved through solution‐phase polymerization of dual‐ended acrylic monomers on prepatterned substrates and surface‐mediated creation of area‐dependent nucleation barriers using adsorption inhibitors and chain terminators, which synergistically modulate surface and bulk free energy of nucleation, respectively. The resulting resist forms a coherent resin film physically adhered to the substrate, while featuring tunable thickness (13–150 nm) and minimal surface roughness (0.91 nm). This method delivers 15 nm linewidth patterning with 99.97% coverage across wafer‐scale arrays within 10 s and demonstrates high compatibility with mainstream thin‐film deposition techniques (e.g., e‐beam evaporation, sputtering, and atomic layer deposition).