A solvent‐assisted grinding method has been used to prepare co‐crystals in substituted dihydropyrimidines (DHPM) that constitutes pharmacologically active compounds. These were characterized using FT‐IR, PXRD, and single‐crystal X‐ray diffraction. In order to explore the possibility of formation of halogen (XB) and hydrogen bonding (HB) synthons in the solid state, co‐crystallization attempts of differently substituted DHPM molecules, containing nitro, hydoxy, and chloro substituents, with different co‐formers, such as 1,4‐diiodo tetrafluorobenzene (1,4 DITFB) and 3‐nitrobenzoic acid (3 NBA) were performed. The XB co‐crystals (C2aXB, C2bXB, and C2cXB) prefer the formation of C−I⋅⋅⋅O/C−I⋅⋅⋅S XB synthon, whereas the HB co‐crystal (C2dHB) is stabilized by N−H⋅⋅⋅O H‐bond formation. Hirshfeld surface analysis revealed that the percentage contribution of intermolecular interactions for XB co‐crystals prefer equal contribution of XB synthon along with HB synthon. Furthermore, the interaction energy was analyzed using energy frameworks, which suggests that their stability, a combination of electrostatics and dispersion, is enhanced through XB/HB in comparison to the parent DHPMs.

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