In order to solve the pollution of heavy metals and organic antibiotic in the water environment, a novel CuBi2O4/calcined ZnAlBi layered double hydroxides (CBO/CLDHs) composite was constructed and prepared via an ultrasonic-assisted calcination method for the adsorption and photocatalysis synergetic effect. Through varying the composition ratio, pH value, initial pollutant concentration and other pollutant interference, the simultaneous removal ability including adsorption and photocatalysis of as-prepared CBO/CLDHs composites for Cr(VI) and tetracycline pollutants was discussed. In particular, the CBO/CLDHs-1/15 composite showed that the removal efficiencies of Cr(VI) (40 mg/L) and tetracycline (40 mg/L) were both above 95%. Meanwhile, the XPS results confirmed that the toxic Cr(VI) was gradually reduced to non-toxic Cr(III) under visible light irradiation. The enhanced adsorption and photocatalytic activity was mainly attributed to the uniform distribution of calcined ZnAlBi layered double hydroxides nanosheets on the CuBi2O4 microrods and the formation of heterojunctions. Moreover, cycle performance results revealed that the CBO/CLDHs-1/15 composite maintained high removal activity and stable structure after 4 photocatalytic cycles, and even showed a good adaptability while applied to the actual water in production and living environments. These results exhibited that the as-prepared CBO/CLDHs-1/15 composite has excellent adsorption and photocatalytic ability for the simultaneous removal of Cr(VI) and tetracycline, with a great potential application in practical waste water treatment field.