A 1D Mo^VMn^III chain compound balanced by {Fe[HC(3,5-Me₂pz)₃]₂}²⁺ dications was prepared. This complex displays a typical single-chain magnet character associated with the Mo^VMn^III chain and a spin crossover phenomenon arising from cationic Fe(II) subunits. The spin crossover behavior tends to slightly affect single-chain magnetic properties at low temperature.