TRIUMF is one of the only laboratories in the world able to produce both lead-203 (203Pb, t1/2= 51.9 h) and212Pb (t1/2= 10.6 h) onsite via its 13 and 500 MeV cyclotrons, respectively. Together,203Pb and212Pb form an element-equivalent theranostic pair that potentiate image-guided, personalized cancer treatment, using203Pb as a single-photon emission computed tomography (SPECT) source, and212Pb for targeted alpha therapy. In this study, improvements to203Pb production were accomplished by manufacturing electroplated, silver-backed thallium (Tl) targets to improve target thermal stability, which allow for higher currents during irradiation. We implemented a novel, two-column purification method that employs selective Tl precipitation (203Pb only) alongside extraction and anion exchange chromatography to elute high specific activity and chemical purity203/212Pb in a minimal volume of dilute acid, without the need for evaporation. Optimization of the purification method translated to improvements in radiolabeling yields and apparent molar activity of lead chelators TCMC (S-2-(4-Isothiocyanatobenzyl)-1,4,7,10-tetraaza-1,4,7,10-tetra(2-carbamoylmethyl)cyclododecane) and Crypt-OH, a derivative of a [2.2.2]-cryptand.