A new generation of low-power high-density information storage would be enabled by the development of ?multiferroic? materials which function at or above room temperature. Such materials are rare, as they require polarisation P to be coupled with spontaneous magnetisation from long-range magnetic ordering M within a single phase material: these properties have antagonistic electronic requirements maing them extremely difficult to couple above room temperature. We are investigating a new approach to combining P and M at high temperatures using octahedral tilt distortions in a layered perovskite to contol structure and magnetism. We aim to characterise a new series of compounds by neutron diffraction so that their physical properties may be optimised on the basis of a detailed understanding of their structures and long-range magnetic ordering.