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Low- and atmospheric-pressure plasma co-polymerisations of binary gas mixtures of C2H4 and NH3 or N2, respectively, were investigated for depositing N-rich plasma polymer coatings for biomedical applications. Deposition kinetics and relevant surface characteristics of resulting plasma polymerised ethylene enriched with nitrogen, PPE:N, coatings were investigated as a function of the gas mixture ratio, X = NH3(N2)/C2H4. Physico-chemical properties of the coatings were determined using a combination of complementary surface-sensitive techniques: for example, total nitrogen concentrations, [N], up to 40 at.% were measured by X-ray Photoelectron Spectroscopy, XPS, while those of primary amines, [NH2], were determined by performing chemical derivatisation followed by XPS analyses. PPE:N films were further characterised by UVVIS Ellipsometry, Near Edge X-ray Absorption Fine Structure Spectroscopy, IR Spectroscopy and by Contact Angle Goniometry measurements. The stability of the coatings was tested, both in terms of water solubility and of ageing in ambient atmosphere. For the latter, selected samples were stored in the laboratory for different durations, in order to assess possible changes in their chemical structures.