Ferrocene (Fc) and tetrathiafulvalene (TTF) moieties were incorporated into novel hybrid molecules of structure FcS(4)TTF(R)(2) (R = CF3 and SMe). [FcS(4)TTF(R)(2)](center dot+) exhibited R-dependent spin-density distribution, and [FcS(4)TTF(CF3)(2)](center dot center dot 2+) showed the coexistence of Fc-centered Fe 3d and TTF-centered pi spins. The solid-state molecular structures in different oxidation states reflect their characteristic spin states.