The invention discloses a Nd and Sm separation method applied to Nd isotopc analysis of a thermal ionization mass spectrum. The method comprises the following steps of sample dissolving, in which a sample is dissolved to obtain a 3mol/L of HNO3 medium sample solution; and chemical separation, in which the sample solution is loaded onto an exchange column which is filled with 1.0ml of TODGA levextrel resin, 10ml 3mol/L of HNO3 is used to wash out basic elements including Fe, Mg, Al, K, Na, Cr, Ti and Ba, 10mL 11mol/L HNO3 is used to wash out Ca, 15ml 2.5mol/L HCl is used to wash out interference elements including La, Ce and Pr, 6mL 2mol/L of HCl is used to analyze Nd, and 5mL 0.5mol/L HCl is used to analyze Sm. According to the method, neodymium and samarium can be separated from a geologic sample by one column, Nd and Sm obtained by separation are high in purity and recovery rate, the method is rapid and efficient, and the flow background is low.