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Bismuth oxide solubility in Bi₂O₃–ZnO–Nb₂O₅ and Bi₂O₃–MgO–Nb₂O₅ (BMN) pyrochlore systems was investigated and the solubility limits were identified. Differences in the solubility behavior between the two Bi-pyrochlore systems investigated were analyzed and explained through crystal chemistry concepts. For the BMN system, the dielectric constant was enhanced, and a systematic shift occurred in the dielectric relaxation loss peak to higher temperatures with increases in the excess bismuth are reported in the BMN system. The relationship between solubility and the shift in the dielectric loss curve was analyzed under the scope of possible relaxation mechanisms.