The adsorbents for water treatment and purification are commonly not recyclable because of the lack of a reagent-less “switch” to readily release the adsorbed compounds. Herein, the interface of Bi2O2CO3 (BOC) nanosheets is designed, synthesized, and modified with citric acid, namely, modified Bi2O2CO3 (m-BOC). The m-BOC is able to selectively adsorb methylene blue (MB) in the dark and the adsorbed MB could be released in the light from m-BOC without the addition of any chemicals. The adsorption mechanism is attributed to the electrostatic attraction between positively charged MB and the negatively charged surface of m-BOC. In contrast, the desorption of MB has resulted from the photo-induced charge redistribution on the surface of m-BOC, which unlocks the coordination bond between m-BOC and the carboxylic group. As a result, BOC is recycled. Such a mechanism was verified by both experimental investigation and DFT calculation. This work provides a promising interfacial engineering strategy for the remediation of dye-polluted water and smart separation in chemical engineering.