Several synthetic techniques are available for the preparation of halogen-bonded adducts, including traditional solvent-evaporation methods and mechanochemistry. With the intention of reducing solvent usage and experimental times, we establish cosublimation as a synthetic technique for preparing halogen-bonded cocrystals, focusing on the C–I···N motif involving nitrogen-containing heterocycles. We selected four common halogen-bond donors (I2, 1,4-diiodobenzene, 1,4-diiodotetrafluorobenzene, 1,3,5-trifluoro-2,4,6-triiodobenzene) and four halogen-bond acceptors (2,3,5,6-tetramethylpyrazine, 1,4-diazabicyclo[2.2.2]octane, 2,2′-bipyridyl, 1-adamantanecarbonitrile), by virtue of their range in volatility, and explored all 16 combinations via the following methods: solvent evaporation, overnight cosublimation in a sealed glass tube using a two-zone furnace, and expedited cosublimation in a vacuum sublimation apparatus. We show that the raw crystals obtained from overnight cosublimation are of suitable quality f...