The interface structure and magnetism of hybrid magnetic tunnel junction-spin filter devices have been investigated and correlated with their transport properties. Magnetic tunnel junctions made of a spinel NiMn2O4 tunnel barrier sandwiched by theoretically predicted half-metallic electrodes, perovskite La0.7Sr0.3MnO3 and spinel Fe3O4, exhibit very high crystalline quality as observed by transmission electron microscopy. Structurally abrupt interfaces allow for the distinct magnetic switching of the electrodes as well as large junction magnetoresistance. The change in the magnetic anisotropy observed at the spinel-spinel interface is indicative of a thin interdiffused magnetically soft interfacial layer. The strong exchange coupling at this interface allows for low background magnetoresistance, and a spin-filter effect with when the barrier is ferrimagnetic. (C) 2008 American Vacuum Society.