Heavy metal pollution is still a major challenge around the world. Traditional treatment methods have unqualified to the sustainable development strategy due to high cost, environment pollution, low efficiency, etc. Cellulose nanofibers (CNF) have a bright application prospect due to rich sources, renewable, high activity, large specific surface area and low density, which has been widely applied in environment, food, agriculture fields for the adsorption of heavy metal in recent years. In this paper, the chemical modification methods of CNF and the application progress of the modified products in the adsorption of heavy metal ions in water system are reviewed. Firstly, the modification of CNF is summarized systematically, including chemical graft modification (carboxylation, amination, hydrophobicity, phosphorylation, sulfonic acid group, aldehyde group, silanization, etc.) and graft copolymerization modification. Secondly, from the aspect of structural design, the application of modified CNF in adsorption of heavy metal ions in water system by different forms such as aerogel, hydrogel and composite membrane is emphatically expounded. Finally, the advantages and disadvantages of CNF-based heavy metal adsorbents are discussed, the limitations and applicability of CNF-based heavy metal adsorbents are pointed out, and the development direction of CNF in the field of heavy metal ion removal in water system is prospected.