Vertically aligned carbon nanofibers partially embedded inside polyurethane (eVACNFs) are proposed as a robust high friction fibrillar material with a compliant backing. Carbon nanofibers with 50–150 nm in diameter and 20–30 μm in length are vertically grown on silicon and transferred completely inside an elastomer by vacuum molding. By using time controlled and selective oxygen plasma etching, fibers are partially released up to 5 μm length. Macroscale friction experiments show that eVACNFs exhibit reproducible effective friction coefficients up to 1. Besides high friction, the proposed fabrication method improves fiber-substrate bond strength, and enables uniform height nanofibers with a compliant backing.