Simultaneous and highly efficient removal of heavy metal cations and oxyanions is significant for both water and soil remediation, but it remains a major challenge due to the complexity. In this work, a novel hybrid of α-FeOOH incorporated carboxylated cellulose nanocrystal (Fe/CNC) is synthesized via a hydrothermal process, which shows improved α-FeOOH dispersion and heavy metal removal capacity. In single adsorbate system, maximum adsorption capacities toward Pb(II), Cd(II), and As(V) by Fe/CNC reach 126.06, 53.07, and 15.80mgg-1, respectively, and the Fe leaching is much lower than that of α-FeOOH. In binary and ternary adsorption systems, simultaneous removal of Pb(II), Cd(II), and As(V) is proved, and the competition and synergy coexist among heavy metals. FTIR and XPS spectra have revealed the synergistic removal mechanism: Pb(II) and Cd(II) are mainly removed by surface complexation with oxygen-containing functional groups on C-CNC and α-FeOOH, and precipitation on the surface of α-FeOOH, while ligand exchange with Fe-OH is responsible for As(V) removal. The soil incubation experiments show that exchangeable and carbonate-bound Pb, Cd, and As are transformed into more stable forms in contaminated soil containing Fe/CNC composites. This work provides a novel composite material for remediation of heavy metal-contaminated environments.