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Hybrid perovskites have generated a great deal of interest because of their potential in photovoltaic applications. However, the toxicity of lead means that there is interest in finding a nontoxic substitute. Bulk single crystals of both cubic CH₃NH₃SnI₃ and CH(NH₂)₂SnI₃ were obtained by using the top‐seeded solution growth method under an ambient atmosphere. Structural refinement, band gap, thermal properties, and XPS measurements of CH₃NH₃SnI₃ and CH(NH₂)₂SnI₃ single crystals are also reported in detail. These results should pave the way for further applications of CH₃NH₃SnI₃ and CH(NH₂)₂SnI₃.