Spin-crossover centres are a fascinating class of molecular switch for which variation of temperature, pressure, light irradiation, magnetic field and chemical environment can be used ti stimulate changes in molecular structure, colour and magnetism. Here we propose a wide range of new spin-crossover systems where cooperativity between switching centres, induced by careful supramolecular design, will lead to advanced molecules and materials having unprecedented host-guest capabilities, magnetic ordering, memory retention and/or exotic multifunctional properties. The work directly targets several fundamental questions in the science of electronic systems and will lead to novel switchable properties worthy of commercial development