Introduction: Radiotherapy of cancer requires both alpha- and beta-particle emitting radionuclides, as these radionuclide types are efficient at destroying different types of tumors. Both classes of radionuclides require a vehicle, such as an antibody or a polymer, to be delivered and retained within the tumor. Polyglutamic acid (pGlu) is a polymer that has proven itself effective as a basis of drug-polymer conjugates in the clinic, while its derivatives have been used for pretargeted tumor imaging in a research setup. trans-Cyclooctene (TCO) modified pGlu is suitable for pretargeted imaging or therapy, as well as for intratumoral radionuclide therapy. In all cases, it becomes indirectly radiolabeled via the bioorthogonal click reaction with the tetrazine (Tz) molecule carrying the radionuclide. In this study, we report the radiolabeling of TCO-modified pGlu with either lutetium-177 (¹⁷⁷Lu), a beta-particle emitter, or actinium-225 (²²⁵Ac), an alpha-particle emitter, using the click reaction between TCO and Tz. Methods: A panel of Tz derivatives containing a metal ion binding chelator (DOTA or macropa) connected to the Tz moiety directly or through a polyethylene glycol (PEG) linker was synthesized and tested for their ability to chelate ¹⁷⁷Lu and ²²⁵Ac, and click to pGlu-TCO. Radiolabeled ¹⁷⁷Lu-pGlu and ²²⁵Ac-pGlu were isolated by size exclusion chromatography. The retention of ¹⁷⁷Lu or ²²⁵Ac by the obtained conjugates was investigated in vitro in human serum. Results: All DOTA-modified Tzs efficiently chelated ¹⁷⁷Lu resulting in average radiochemical conversions (RCC) of >75%. Isolated radiochemical yields (RCY) for ¹⁷⁷Lu-pGlu prepared from ¹⁷⁷Lu-Tzs ranged from 31% to 55%. TLC analyses detected <5% unchelated ¹⁷⁷Lu for all ¹⁷⁷Lu-pGlu preparations over six days in human serum. For ²²⁵Ac chelation, optimized RCCs ranged from 61 ± 34% to quantitative for DOTA-Tzs and were quantitative for the macropa-modified Tz (>98%). Isolated radiochemical yields (RCY) for ²²⁵Ac-pGlu prepared from ²²⁵Ac-Tzs ranged from 28% to 51%. For 3 out of 5 ²²⁵Ac-pGlu conjugates prepared from DOTA-Tzs, the amount of unchelated ²²⁵Ac stayed below 10% over six days in human serum, while ²²⁵Ac-pGlu prepared from macropa-Tz showed a steady release of up to 37% ²²⁵Ac. Conclusion: We labeled TCO-modified pGlu polymers with alpha- and beta-emitting radionuclides in acceptable RCYs. All ¹⁷⁷Lu-pGlu preparations and some ²²⁵Ac-pGlu preparations showed excellent stability in human plasma. Our work shows the potential of pGlu as a vehicle for alpha- and beta-radiotherapy of tumors and demonstrated the usefulness of Tz ligation for indirect radiolabeling.