These findings suggest that achieving desired polar structures requires precise control over solute-solvent interactions during nucleation and crystal growth. Subtle variations in solvent choice and crystallization conditions can significantly influence the formation of specific polymorphs, offering a potential strategy to tailor material properties. Given the inherent complexities of polymorph formation, advanced methodologies such as crystal structure prediction (CSP) are essential for accurate predictions and design of targeted materials. Future studies should focus on refining the understanding of solvent effects and crystallization parameters to enable the deliberate manipulation of polymorph formation. It is therefore important to clarify that the primary objective of this study is not to predict the exact structure of polar cocrystals. Instead, our objective is to establish a robust, data-driven framework that integrates ML techniques with HT automation to streamline the screening and discovery process for polar organic cocrystals.