In this chapter, selected results obtained so far on Fe(II) spin crossover compounds of 1,2,4-triazole, isoxazole and tetrazole derivatives are summarized and analysed. These materials include the only compounds known to have Fe(II)N(6) spin crossover chromophores consisting of six chemically identical heterocyclic ligands. Particular attention is paid to the coordination modes for substituted 1,2,4-triazole derivatives towards Fe(II) resulting in polynuclear and mononuclear compounds exhibiting Fe(II) spin transitions. Furthermore, the physical properties of mononuclear Fe(II) isoxazole and 1-alkyl-tetrazole compounds are discussed in relation to their structures. It will also be shown that the use of alpha,beta- and alpha,omega-bis(tetrazol-1-yl)alkane type ligands allowed a novel strategy towards obtaining polynuclear Fe(II) spin crossover materials.