Zero-shot Image Captioning (ZIC) increasingly utilizes synthetic datasets generated by text-to-image (T2I) models to mitigate the need for costly manual annotation. However, these T2I models often produce images that exhibit semantic misalignments with their corresponding input captions (e.g., missing objects, incorrect attributes), resulting in noisy synthetic image-caption pairs that can hinder model training. Existing dataset pruning techniques are largely designed for removing noisy text in web-crawled data. However, these methods are ill-suited for the distinct challenges of synthetic data, where captions are typically well-formed, but images may be inaccurate representations. To address this gap, we introduce SynC, a novel framework specifically designed to refine synthetic image-caption datasets for ZIC. Instead of conventional filtering or regeneration, SynC focuses on reassigning captions to the most semantically aligned images already present within the synthetic image pool. Our approach employs a one-to-many mapping strategy by initially retrieving multiple relevant candidate images for each caption. We then apply a cycle-consistency-inspired alignment scorer that selects the best image by verifying its ability to retrieve the original caption via image-to-text retrieval. Extensive evaluations demonstrate that SynC consistently and significantly improves performance across various ZIC models on standard benchmarks (MS-COCO, Flickr30k, NoCaps), achieving state-of-the-art results in several scenarios. SynC offers an effective strategy for curating refined synthetic data to enhance ZIC.