The amino-functionalised ferrocene derivative FcCH2CH2NH2 [Fc = Fe(eta-C5H5)(eta-C5H4)] has been intercalated under mild conditions into both single-crystal and microcrystalline samples of the layered host lattices MoO3, 2H-TaS2, and alpha-Zr(HPO4)2.H2O. The X-ray powder patterns for the new intercalates have been indexed and yield interlayer lattice expansions of 13.09, 5.89 and 14.54 angstrom, respectively. The large interlayer expansions of 13.09 and 14.5 angstrom observed for the intercalates of both MoO3 and alpha-Zr(HPO4)2.2H2O suggest the formation of a bilayer of guest molecules within these host lattices. The Fe-57 Mossbauer spectrum of MoO3(FcCH2CH2NH2)0.36 exhibits a quadrupole doublet with an isomer shift delta-Fe = 0.442 mm s-1 and quadrupole splitting DELTA = 2.344 mm s-1, indicating the presence of unoxidised ferrocene molecules within the oxide layers. Solid-state C-13 CP-MAS NMR spectra of MoO3(FcCH2CH2NH2)0.36 are consistent with the existence of both neutral FcCH2CH2NH2 and FcCH2CH2NH3+ moieties within the host. In addition, the changes in the electronic structure of MoO3 that accompany the intercalation of FcCH2CH2NH2 have been investigated by solid-state photoelectron spectroscopy.