This study explores the suitability of microfibrillated cellulose (MFC) films as a substrate for printing electrically conductive structures and multilayer electronic structures such as organic field effect transistors. Various MFC qualities were tested, including mechanically produced MFC, 2,2,6,6-tetramethylpiperidinyl- 1-oxyl pre-treated MFC and carboxymethylated- MFC. The films differed significantly with respect to the surface structure. In addition, the carboxymethylated-MFC films were surface modified with hexamethyldisilazane (HMDS) to reduce the water-wettability of the films, and thus, improve the print resolution of the inkjet-printed silver (Ag) nanoparticles. The Ag-particles (diameter>50 nm) were printed on the HMDS-modified films, which were mainly composed of nanofibrils with diameters >20 nm. The effect of surface roughness and surface chemical characteristics on the ink spreading and print resolution of the Ag-structures was explored. It was demonstrated that organic transistors operating at low voltages can be fabricated on nano-engineered MFC films.