A new 3-fold symmetric molecular host, tris(isonicotinoyl)cyclotriguaiacylene, has been synthesized from cyclotriguaiacylene and isonicotinoyl chloride hydrochloride in 70% yield. Its crystal structure shows dimerization of the host molecules into a capsule-like arrangement. When reacted with Ag[CO(C2B9H11)(2)], the host forms a 1-D [ML2](n) coordination polymer, which assembles into a 2-D interwoven network through a similar dimerization of the host moieties around acetonitrile guests. Thus, the network structure represents an elegant example whereby the solid state structure of the building blocks is echoed in the resulting supramolecular assembly. The 2-D sheets are further stabilized by pi(...)pi stacking interactions between pyridyl donors of alternate 1-D coordination polymers.