A new sequential cloud point extraction (CPE) procedure was developed and validated for the determination of 210Pb and 210Po by ICP-MS/MS and alpha spectrometry, respectively. Two distinct CPE systems using 4',4''(5'')-di-tert-butyldicyclohexano-18-crown-6 and N,N,N',N'-tetraoctyldiglycolamide as chelating agents were performed sequentially on the same sample. Method detection limits of 13 and 3.5 mBq L-1, were achieved for 210Pb and 210Po, respectively. The sequential approach shows its outstanding versatility and proficiency to rapidly extract, detect, and quantify both radionuclides in various matrices for a wide range of activities.