We find that nitrogen plasma treatment of micro/nanofibrillated cellulose films increases wettability of the surface by both liquid polar water and nonpolar hexadecane. The increased wetting effect is more pronounced in the case of polar liquid, favouring the use of plasma treated micro/nanofibrillated cellulose films as substrates for a range of inkjet printing including organic-based polar-solvent inks. The films were formed from aqueous suspensions of progressively enzymatic pretreated wood-free cellulose fibres, resulting in increased removal of amorphous species producing novel nanocellulose surfaces displaying increasing crystallinity. The mechanical properties of each film are shown to be highly dependent on the enzymatic pretreatment time. The change in surface chemistry arising from exposure to nitrogen plasma is revealed using X-ray photoelectron spectroscopy. That both polar and dispersive surface energy components become increased, as measured by contact angle, is also linked to an increase in surface roughness. The change in surface free energy is exemplified to favour the trapping of photovoltaic inks.