Photocatalytic technology is the recent investigation focus because of the wide applications in sewage disposal and new energy generation. In this paper, the optical and photocatalytic properties of TiO2 NTAs were enhanced by the hydrothermal deposition of CuBi2O4 by regulating the precursor concentration. The results indicated that the precursor concentration played remarkable influences on the morphology and photocatalytic ability. The mild reagent concentration was in favor of super-thin CuBi2O4 nanosheet formation. CuBi2O4/TiO2 NTAs with high reagent concentration exhibited high photocurrent and hydrogen production, and showed outstanding performance in the removal of organic dyes and heavy metal ions. The free radical production and the photocatalytic progress were introduced in detail. The high photocatalytic activity exhibits prospective foreground in industrial waste water treatment and novel energy resource development.