The syntheses, structures, and magnetic properties of a family of bimetallic anilate-based compounds with inserted spin-crossover cationic complexes are reported. The structures of 1-4 present a two-dimensional anionic network formed by Mn(II) and Cr(III) ions linked through anilate ligands with inserted [Fe-III(sal(2)-trien)](+) (1), [Fe-III(4-OH-sal(2)-trien)](+) (2), [Fe-III(sal(2)-epe)](+) (3), or [Fe-III(5-Cl-sal(2)-trien)](+) (4) complexes. The structure of 5 is formed by anionic [(MnClCrIII)-Cl-II-Cr-2(Cl(2)An)(3)](3-) chains surrounded by [Fe-II(tren(imid)(3))](2+), Cl-, and solvent molecules. The magnetic properties indicate that 1-4 undergo a long-range ferrimagnetic ordering at ca. 10 K. On the other hand, the inserted Fe(III) cations remain in the low-spin (in 4) or high-spin state (in 1, 2, and 3). In the case of 5, half of the inserted Fe(II) cations undergo a complete and gradual spin crossover from 280 to 90 K that coexists with a magnetic ordering below 2.5 K.