Novel mono- and trinuclear iron(III) complexes with mixed ligands, Fe-III(acac) (N-PhO-sal)(MeOH) 1. and Fe-3(III)(acac)(N-PhO-sal)(4) 2 have been prepared and characterized, where acacH and N-PhON-salH denote acetylacetone and N-2-hydroxyphenyl-salicylideneamine, respectively. The variable temperature magnetic susceptibilities (2-350 K) for complex 2 indicate that there is an intramolecular antiferromagnetic interaction among the iron(III) ions, and that spin-crossover behavior may take place from S = 5/2, 5/2 and 5/2 ground states to S = 1/2, 5/2 and 1/2 (Fe1, Fe2 and Fe1*) near 60 K and below.