The engineering of biomaterial surfaces and scaffolds for specific biomedical and clinical application is of growing interest. Certain functionalised surfaces can capture and deliver bioactive molecules, such as growth factors (GF), enhancing the clinical efficacy of such systems. With a custom-made plasma polymerisation reactor described here we have developed bioactive polymer coatings based on poly(ethyl acrylate) (PEA). This remarkable polymer unfolds fibronectin (FN) upon adsorption to allow the GF binding region of FN to sequester and present GFs with high efficiency. We systematically evaluate process conditions and their impact on plasma polymerised PEA coatings and characterise the effect of plasma power and deposition time on thickness, wettability and chemical composition of the coatings. We demonstrate that functional substrate roughness can be maintained after deposition of the polymer coatings. Importantly, we show that coatings deposited at different conditions all maintain a similar or better bioactivity than spin coated PEA references. We show that in PEA plasma polymerised coatings FN assembles into nanonetworks with high availability of integrin and GF binding regions that sequester bone morphogenetic protein-2 (BMP-2). We also report similar mesenchymal stem cell adhesion behaviour, as characterised by focal adhesions, and differentiation potential on BMP-2 coated surfaces, regardless of plasma deposition conditions. This is a potent and versatile technology that can help facilitate the use of GFs in clinical applications.