Three novel stilbene derivatives with high two-photon cross-section are designed and synthesized as two-photon chromophores. Three-dimensional (3D) optical data storage experiments are carried out by two-photon photobleaching with a femtosecond laser in three stilbene derivatives doped polymethylmethacryate film. Research on the two-photon photobleaching ability of three two-photon chromophores shows that the chromophore with larger two-photon cross-section could be photobleached at lower excitation power. The effects of excitation power on two-photon fluorescence behaviors are also analyzed. The characters of optical data storage reveal that the resolution in two-photon photobleaching could be increased by lowing excitation power when exposure time is kept the same or by lowing exposure time when excitation power is kept the same. However, larger excitation power is often used to obtain high data storage rate. Two-photon writing and two-photon reading experiment realizes 3D ultrahigh optical data storage with a theoretical storage density of 14 Gbit/cm3 in doped film under higher excitation power (13.4 mW) and shorter exposure time (20 ms). The cubic dependence of two-photon photobleaching dynamics on excitation power indicates that the mechanism of two-photon photobleaching concerns the joint action of three photons.