A series of diarylethene derivatives with two-photon absorption was designed and synthesized. The nonlinear properties of two-photon induced fluorescence of the compounds were examined. A strategy for the design of molecules with large two-photon absorption (TRA) was developed. These compounds were also successfully applied in two-photon three-dimensional (3D) optical data storage based on single beam two-photon femtosecond writing and one-photon fluorescence reading.