Industrial wastewater containing hexavalent chromium Cr(VI) and phosphate poses a great threat to human health and the aquatic ecological environment. In this study, a novel La(OH)3- and CaO2-fabricated CNT (La-Ca-CNT) material was developed for the simultaneous and highly effective removal of aqueous Cr(VI) and phosphate. Characterization results showed that synergistic effects existed between the CNT support and La and Ca species. La-Ca-CNT showed high phosphate and Cr(VI) removal rates in acidic conditions with high stability. Kinetic study suggested that the fast adsorption of phosphate on La-Ca-CNT was controlled by intraparticle diffusion. The removal of Cr(VI) and phosphate interacted with each other, and the removal of Cr(VI) went through a slow-fast-slow reaction, reaching a Cr(VI) removal rate of over 97% within 180min. La-Ca-CNT had a high phosphate adsorption capacity (174.3mg/g), and over 70% of the adsorbed phosphate could be recovered. The presence of co-existing anions showed negative effects on phosphate adsorption but negligible effects on Cr(VI) reduction, while organic carbon in natural water showed no effect on phosphate and Cr(VI) removal. A mechanistic study revealed that phosphate was removed by physical-chemical adsorption (outer-sphere complexation and ligand exchange) over La-Ca-CNT, while Cr(VI) was reduced by H2O2 generated from CaO2 or directly by surface CaO2.