Cellulose　nanofibrils　(CNFs)　are　derived　from　biomass　and　have　significant　potential　as　fossil-based　plastic　alternatives　used　in　disposable　electronics.　Controlling　the　nanostructure　of　fibrils　is　the　key　to　obtaining　strong　mechanical　properties　and　high　optical　transparency.　Vacuum　filtration　is　usually　used　to　prepare　the　CNFs　film　in　the　literature;　however,　such　a　process　cannot　control　the　structure　of　the　CNFs　film,　which　limits　the　transparency　and　mechanical　strength　of　the　film.　Here,　direct　ink　writing　(DIW),　a　pressure-controlled　extrusion　process,　is　proposed　to　fabricate　the　CNFs　film,　which　can　significantly　harness　the　alignment　of　fibrils　by　exerting　shear　stress　force　on　the　filaments.　The　printed　films　by　DIW　have　a　compact　structure,　and　the　degree　of　fibril　alignment　quantified　by　the　small　angle　X-ray　diffraction　(SAXS)　increases　by　24　%　compared　to　the　vacuum　filtration　process.　Such　a　process　favors　the　establishment　of　the　chemical　bond　(or　interaction)　between　molecules,　therefore　leading　to　considerably　high　tensile　strength　(245　+/-　8　MPa),　elongation　at　break　(2.2　+/-　0.5　%),　and　good　transparency.　Thus,　proposed　DIW　provides　a　new　strategy　for　fabricating　aligned　CNFs　films　in　a　controlled　manner　with　tunable　macroscale　properties.　Moreover,　this　work　provides　theoretical　guidance　for　employing　CNFs　as　structural　and　reinforcing　materials　to　design　disposable　electronics.