We analyzed real-world clinical outcomes of sequential α-/β-emitter therapy for metastatic castration-resistant prostate cancer (mCRPC). We assessed safety and overall survival in 26 patients who received Lu-prostate-specific membrane antigen ligand (Lu-PSMA) after Ra in the ongoing noninterventional REASSURE study (Ra α-Emitter Agent in Nonintervention Safety Study in mCRPC Population for Long-Term Evaluation; NCT02141438). Patients received Ra for a median of 6 injections and subsequent Lu-PSMA for a median of 3.5 mo (≥ the fourth therapy in 69%). The median time between Ra and Lu-PSMA treatment was 8 mo (range, 1-31 mo). Grade 3 hematologic events occurred in 9 of 26 patients (during or after Lu-PSMA treatment in 5/9 patients; 8/9 patients had also received docetaxel). Median overall survival was 28.0 mo from the Ra start and 13.2 mo from the Lu-PSMA start. Although the small sample size precludes definitive conclusions, these preliminary data, especially the Lu-PSMA treatment duration, suggest that the use of Lu-PSMA after Ra is feasible in this real-world setting.