Homoleptic and heteroleptic cylinder‐shaped poly‐NHC metallosupramolecular assemblies [Ag (L) ](BF ) have been prepared by control of the shape, size, and electronic properties of disk‐shaped trisimidazolium salts of type H ‐L(BF ) . Both imidazolium salts with an electron‐deficient triazine backbone H ‐A(BF ) or an electron‐rich benzene backbone H ‐D(BF ) have been employed. Reaction of H ‐A(BF ) or H ‐D(BF ) with Ag O yield trinuclear homoligand complexes [Ag (L) ](BF ) (L=A, D).