A novel process for realizing uniform and controllable doping of Si3N4 single crystal dimension nano materials by organic precursor co-pyrogenation comprises the following concrete steps: (1) ball milling mixing: ball milling and mixing homogeneously two organic precursors (polysilazane and aluminium isopropoxide ) according to different proportions; (2) low temperature cross linkage solidification: cross linkage solidifying after mixing homogeneously to get non-crystalline solids; (4) high-energy ball milling pulverizing: filled the non-crystalline solids to a nylon resin milling tank, introducing a catalyzer therein, and dry method ball milling pulverizing them in a high-energy globe mill; (4) high temperature thermal decomposition: after the high-energy ball milling, thermal decompositing the mixture. Different the traditional doping process, said novel process can realize the regulation and design of uniform doping of Si3N4 single crystal dimension nano material in molecular level by simply regulating the proportionality of two organic precursors, and then realize the regulation of performances such as actinoelectricity of Si3N4 single crystal dimension nano materials. Said process is hopeful to become a general process for realizing controllable doping of single crystal low dimension nano materials.