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Blood-contacting devices have emerged in the 21st century as the go-to clinical treatment for severe cardiovascular diseases. Due to their poor hemocompatibility, many coatings have been developed to improve their biocompatibility with limited success due to the lack of robustness in biomolecule conjugation. In this paper, we propose a new self-protonating, plasma polymerized, superimposed multi-layered nanoreservoir coating for immobilization of charged biomolecules, and demonstrated its high surface charge density, loading capabilities and most importantly, bioactivity retention of biomolecules. Using heparin as a model therapeutic, we demonstrated the advantages of our coating strategy through in vitro and ex vivo means. Our findings will open a new path in clinical device coating strategies in biomolecule functionalization to benefit many patients worldwide.