As for traditional adsorbents, regeneration is commonly carried out with the aid of acid or alkali to improve the efficiency of water treatment. In this work, a facile and versatile urea-assisted solvothermal procedure was employed to synthesize a new type of adsorbents with unique photo-regeneration capability. The zinc alkoxides in our design can effectively modulate the bandgap of ZnO from 3.27 to 2.49 eV, and therefore they can be degraded under ultraviolet irradiation with the help of ZnO photocatalyst. Moreover, these long-chain zinc alkoxides are of superior adsorption capability with a maximum adsorption capacity of 200.3 mg g(-1) and an initial adsorption rate of 3.6 mg g(-1) min(-1) at 298 K, due to their abundant surface groups to induce physisorption as well as chemisorption for Cr(VI) species in waste water. After Cr(VI) adsorption, the as-designed adsorbent can be facilely regenerated with ultraviolet irradiation in warm water. It is anticipated that this new design of adsorbent will shed new light on the development of next generation of adsorbents in water-treatment field.