Ultrathin Organic and polymer films used for organic electronics can be prepared by wet spin coating, polymer grafting, chemical and physical vapor depositions, etc. It is important to control the microstructure and nanostructure of such films not only to control adhesion but also charge carrier and hole transport. In Organic electronic including flexible displays, the preparation of such films enables a key function in controlling device performance and stability. Herewith, we report a combination of polymer surface grafting protocols produces by electrochemical crosslinking and vapor deposition methods to nanostructure the surface leading to better device performance. This can also be achieved by patterning and controlling the surface adhesion forces between the layers. The hole transport and injection layers can also be matched with the ability to prepare more efficient devices through evaporation techniques. A focus is made on using polycarbazole based hole-transport materials.