This invention relates a method of six-dimensional optical multilayer storage using two-photon absorption writing, erasing and optical coherence tomography reading and the apparatus designed based on this method. The invented system stores data in three spatial dimensions plus three physical dimensions of wavelength, intensity and polarization. It has large storage capacity of over 32 Tbytes per DVD sized disk and ultrafast reading speed of over 25 Gbits/s with high signal-to-noise ratio of over 76 dB. The larger capacity of over 1 Pbyte per disk is potential. Furthermore, the invented system has relatively simple optical structure, easy light manipulation for addressing the storage cell and high compatibility with the CDs and DVDs. It is an actually practicable optical large capacity storage technology.