The differences in magnetic properties of metal-based nanometric assemblies are due to distinct contributions from host-guest interactions, structural integrity, and magnetic interactions. To disentangle these contributions, it is necessary to control the self-assembly process that forms these entities. Herein we study the effect of host-to-guest ratios to identify remarkably different structural magnetic contributions of C-methylpyrogallol[4]areneCferrocene/(PgC(1))(2)subset of Fc dimers vs (PgC(1))(3)CFc nanotubes. At low temperature, a weak anti-ferromagnetic alignment is observed, suggesting a weak dipolar interaction between Fc guest moieties within adjacent dimers or tubes. Also, differences are observed between magnetic atom occupancy as a function of guest (PgC(1)subset of Fc tube/dimer) versus magnetic atom occupancy within the framework wall (PgC(3)Ni hexamer/dimer). Identification of the role of the framework shape and metal metal distances in the crystal lattice opens up unparalleled prospects for materials engineering.