Graphene-like SC3N4 was prepared to phtocatalytically eliminate UO22+ pollutant. Weakening planar hydrogen bonding of g-C3N4 can obtain graphene-like structure. Graphene-like structure modified the electronic structures of g-C3N4. SC3N4 showed remarkable performance in the photocatalytic reduction of UO22+. The good activity of SC3N4 was explored both experimentally and theoretically.