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Group V doping in CdSeTe device can improve power conversion efficiency (PCE) and device stability. Arsenic (As) incorporation into CdSeTe has been demonstrated via both in situ and ex situ techniques; however, optimizing the back contact for group V‐doped CdSeTe devices remains a critical challenge. Here, solution‐processed arsenic chalcogenides (i.e., As₂Te₃and As₂Se₃) as dual‐role materials, serving as both dopants and back‐contact materials for high‐efficiency CdSeTe devices, are investigated. During the formation of the back contact, a portion of the arsenic chalcogenides diffuses into the CdSeTe absorber, facilitating p‐type doping. The remaining materials forms a stable back‐contact layer that facilitate carrier collection and reducing recombination losses at the CdSeTe back surface. Particularly, CdSeTe device employing Te rich As₂Te₃layer as the dopant and back‐contact materials achieves a PCE of 18.34%, demonstrating the dual functionality of solution‐processed arsenic chalcogenides in simultaneously doping the absorber and optimizing charge extraction. This solution based cost‐effective As doping approach offers a promising pathway for advancing CdSeTe photovoltaic technology.