As a good alternative to natural bers and petroleum-derived bers, Lyocell bers draw increasing interests owing to its advantages of sustainable forest source, low carbon emission, high strength and comfort. However, Lyocell exhibits signi cant brillation behavior under friction, which seriously reduce product quality and limit its further development. Herein, dual crosslinking networks were innovatively constructed in Lyocell cellulose structure to enhance the interaction of cellulose macromolecular chains. Bifunctional reactive dyes were rstly loaded in cellulose chains to form a primary crosslinking network.Then, the cellulose interaction in Lyocell skin layer was further enhanced after the coating by watersoluble cationic isocyanate polymer. The mechanism was determined and results showed that durable dual crosslinking networks were formed in Lyocell skin-core structure. Dye molecules could form crosslinking structure in both of core and skin layer, and cationic polymer mainly existed on the ber skin layer to construct enhanced crosslinked network. From scanning electron microscope observation, brillation behavior of Lyocell bers was effectively prevented by dual crosslinking networks. Meanwhile, the durability was evaluated, showing that the treated fabric maintained good anti-brillation performance after washing for 50 times. Furthermore, the interaction of dyes and bers was also enhanced by the cationic polymer via electrostatic attraction force, realizing high dye utilization e ciency. Therefore, the method possesses great potential in promoting the application of Lyocell bers in greener textile.