A titanyloxyphthalocyanine crystal to be used as a charge generation material for an electrophotographic photoreceptor, having a maximum diffraction intensity observed at Bragg angle (2 .theta.) of 9.6.degree..+-.0.2.degree. and clear peaks of diffraction intensity observed at 7.22.degree..+-.0.2.degree., 9.60.degree..+-.0.2.degree., 11.60.degree..+-.0.2.degree., 13.40.degree..+-.0.2.degree., 14.88.degree..+-.0.2.degree.,18.34.degree..+-.0.2.degree., 23.62.degree..+-.0.2.degree., 24.14.degree..+-.0.2.degree., and 27.32.degree..+-.0.2.degree., respectively, in an X-ray diffraction spectrum obtained by performing an x-ray diffraction method using CuK.alpha. as a source of radiation. A method for preparing the crystal includes dispersing a predetermined amount of amorphous titanyloxyphthalocyanine in an aqueous solution in which ionic substances are dissolved, under mechanical force at a temperature of under 50.degree. C., to obtain a mixture composed of a fine dispersion of titanyloxyphthalocyanine; adding a non-aqueous organic solvent to the mixture to shift the fine dispersion of titanyloxyphthalocyanine from an aqueous phase to a non-aqueous organic solvent phase; and removing the non-aqueous organic solvent phase to obtain a pellet of titanyloxyphthalocyanine crystal.