This work was financially supported by Industry Research Special Funds for Public Welfare Project of China (201404604), Hunan Provincial Natural Science Foundation (2015JJ2203), Research Foundation of Education Bureau of Hunan Province (15K151), and Hunan Provincial Innovation Foundation for Postgraduate (CX2014A013) from China. The authors sincerely thank Rick Reiner for preparing and supplying TEMPO oxidized cellulose nanofibrils. The authors gratefully acknowledge Jane O’Dell and Nancy Ross Sutherland for DMTA and water contact angle tests, respectively. Benjamin Treml is kindly acknowledged for help with tensile and UV–vis transmittance tests. Thanks also to Neil Gribbins for technical and editorial assistance.