The power conversion efficiency of colloidal PbS‐quantum‐dot (QD)‐based solar cells is significantly hampered by lower‐than‐expected open circuit voltage (VOC). The VOC deficit is considerably higher in QD‐based solar cells compared to other types of existing solar cells due to in‐gap trap‐induced bulk recombination of photogenerated carriers. Here, this study reports a ligand exchange procedure based on a mixture of zinc iodide and 3‐mercaptopropyonic acid to reduce the VOC deficit without compromising the high current density. This layer‐by‐layer solid state ligand exchange treatment enhances the photovoltaic performance from 6.62 to 9.92% with a significant improvement in VOC from 0.58 to 0.66 V. This study further employs optoelectronic characterization, X‐ray photoelectron spectroscopy, and photoluminescence spectroscopy to understand the origin of VOC improvement. The mixed‐ligand treatment reduces the sub‐bandgap traps and significantly reduces bulk recombination in the devices.

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