Incorporating visible light into sulfide oxidation is an emerging desirable strategy to produce versatile sulfoxides. We introduce the design and synthesis of multilayered wrinkled C3N4 nanosheets and demonstrate their unprecedented sulfide oxidation activity. Due to the wrinkled surfaces with a large SBET (208.6 m(2)g(-1)), wrinkled C3N4 nanosheets exhibit a sensitive optical response, facilitating the electron photoexcition. Layer structure confinement enables robust e(-)-h(+) interactions and valid photoexcited excitons formation, allowing rapid O-1(2) reactive species production. Integrating the sensitive optical response with robust e(-)-h(+) interactions, photoexcited electrons and excitons are jointly produced, giving large yields of center dot O-2 and O-1(2) reactive species that are conductive to center dot O-2 and O-1(2) cocatalysis with an activity that is up to 33-fold that of bulk C3N4. In the cocatalysis mechanism, both center dot O-2 and O-1(2), can produce peroxysulfoxide intermediates, resulting in target sulfoxides. This is the first report on sulfide oxidation via center dot O-2 and O-1(2) cocatalysis and a promising study on catalyst exploitation for high-efficiency and high-selectivity production process. (C) 2019 Elsevier Inc. All rights reserved.