Composite UiO-66/nanocellulose aerogels with hierarchical pores and low density were prepared through a self-crosslinking method. The nanocellulose acted as the structural skeleton supporting and dispersing the UiO-66 particles. The micropore and accessibility of UiO-66 were well-preserved, making the composite aerogels ideal sorbents for water purification. The composite aerogels demonstrated high adsorption ability towards both anionic methyl orange (71.7 mg g(-1)) and cationic methylene blue (51.8 mg g(-1)). This work holds a promise to rational design and fabrication of MOF monoliths through group linkage.