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Enabling and understanding new methodologies to fabricate molecular assemblies driven by intermolecular interactions is fundamental in chemistry. Such forces can be used to control crystal growth and enable surface-confinement of these materials, which remains challenging. Here we demonstrate for the first time, a solvent-free on-surface crystal-to-co-crystal conversion process driven by halogen bonding (XB). By exposing a polycrystalline organic material, consisting of a XB-acceptor moiety, to the vapors of a complementary XB-donor compound, the corresponding halogen-bonded co-crystals were formed. Furthermore, we demonstrate that this approach can also be utilized for non-crystalline materials to afford surface-confined organic composites. Our stepwise vapor-based approach offers a new strategy for the formation of hybrid supramolecular materials. [ABSTRACT FROM AUTHOR]