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Ti3CNTx MXenes with unique electrical conductivity can be widely applied for supercapacitors and electromagnetic shielding. However, its relatively low-yield quatary nitrogen-containing Ti3AlCN ceramics precursor (less than 50％), due to the inevitable Al segregation during the synthesizing process, significantly hindered its widely commercial applications. Herein, we employed the controllable AlN-oversaturation precursor strategy to precisely tune the phase transition point of quatary Ti3AlCN ceramics to obtain high-yield Ti3AlCN precursor for the purpose of high conductivity Ti3CNTx MXenes. Combined energy dispersive X-ray spectrometer (XRD) with X-ray photoelectron spectroscopy (XPS) characterizations, the yield of the quatary nitrogen-containing Ti3AlCN ceramics was evidently proved to be up to 70％, which is 1.4 times than that of previously reported works. Such relatively high-yield quatary Ti3AlCN is mainly ascribed to the elimination of Al segregation. Based on it, we further developed accordion-like two-dimensional (2D) MXene via hydrofluoric acid etch and vacuum freeze-dry. This novel accordion-like 2D Ti3CNTx MXene possesses high electrochemical capacitive properties (209 F/g). Therefore, this controllable AlN-oversaturation precursor strategy will pave a way to exploit costly high-yield MAX ceramics precursor for high conductivity MXenes and also play a powerful role in promoting their practical applications including electrical and magnetic engineering fields.