Uniform bismuth oxide (Bi2O3) and bismuth subcarbonate ((BiO)2CO3) nanotubes were successfully synthesized by a facile solvothermal method without the need for any surfactants or templates. The synergistic effect of ethylene glycol (EG) and urea played a critical role in the formation of the tubular nanostructures. These Bi2O3 and (BiO)2CO3 nanotubes exhibited excellent CrVI-removal capacity. Bi2O3 nanotubes, with a maximum CrVI-removal capacity of 79 mg g−1, possessed high removal ability in a wide range of pH values (3–11). Moreover, Bi2O3 and (BiO)2CO3 nanotubes also displayed highly efficient photocatalytic activity for the degradation of RhB under visible-light irradiation. This work not only demonstrates a new and facile route for the fabrication of Bi2O3 and (BiO)2CO3 nanotubes, but also provides new promising adsorbents for the removal of heavy-metal ions and potential photocatalysts for environmental remediation.