A series of high specific activity accelerator-produced radionuclides in no-carrier-added (NCA) form, for uses in metabolic radiotherapy and for PET, has been investigated and produced at JRC-Ispra Cyclotron Laboratory. In this study we present, in particular, the NCA 211At/211gPo (LET = 130 eV.nm-1, t1/2= 7.214 h), produced by 209Bi(α,2n) reaction, with internal spike of gamma emitter 210At (e.g. negligible amount of 210Po as radiotoxic long-lived impurity), for high-LET targeted radiotherapy and immunoradiotherapy. A selective radiochemical separation, based on liquid/liquid extraction, of At radionuclides from Bi target and Po impurities has been developed. High resolution gamma, X and alpha spectrometric techniques have been adopted for quality controls of different radiochemical fractions.