This review summarizes the preparation methods of cellulose nanofibrils (CNFs) and the progress in the research pertaining to their surface modification. Moreover, the preparation and surface modification of nanocellulose were comprehensively introduced based on the existing literature. The review focuses on the mechanical treatment of cellulose, the surface modification of fibrillated fibers during pretreatment, the surface modification of nanocellulose and the modification of CNFs and their functional application. In the past five years, research on cellulose nanofibrils has progressed with developments in nanomaterials research technology. The number of papers on nanocellulose alone has increased by six times. However, owing to its high energy consumption, high cost and challenging industrial production, the applications of nanocellulose remain limited. In addition, although nanofibrils exhibit strong biocompatibility and barrier and mechanical properties, their high hydrophilicity limits their practical application. Current research on cellulose nanofibrils has mainly focused on the industrial production of CNFs, their pretreatment and functional modification and their compatibility with other biomass materials. In the future, with the rapid development of modern science and technology, the demand for biodegradable biomass materials will continue to increase. Furthermore, research on bio-based nanomaterials is expected to advance in the direction of functionalization and popularization.

Because of its non-toxic, pollution-free, and low-cost advantages, environmentally-friendly packaging is receiving widespread attention. However, using simple technology to prepare environmentally-friendly packaging with excellent comprehensive performance is a difficult problem faced by the world. This paper reports a very simple and environmentally-friendly method. The hydroxyl groups of cellulose nanofibrils (CNFs) were modified by introducing malic acid and the silane coupling agent KH-550, and the modified CNF were added to cassava starch as a reinforcing agent to prepare film with excellent mechanical, hydrophobic, and barrier properties. In addition, due to the addition of malic acid and a silane coupling agent, the dispersibility and thermal stability of the modified CNFs became significantly better. By adjusting the order of adding the modifiers, the hydrophobicity of the CNFs and thermal stability were increased by 53.5% and 36.9% ± 2.7%, respectively. At the same time, the addition of modified CNFs increased the tensile strength, hydrophobicity, and water vapor transmission coefficient of the starch-based composite films by 1034%, 129.4%, and 35.95%, respectively. This material can be widely used in the packaging of food, cosmetics, pharmaceuticals, and medical consumables.