A reversible magnetic change in response to external stimuli is a desired function of molecular magnetic materials. The magnetic change induced by a change in the intrinsic spin is significant because the magnetic change is inevitable and could become drastic. In this study, we demonstrate a reversible magnetic change closely associated with electronic state modulations, as well as structural modifications realized by solvation/desolvation cycles of a magnetic sponge. The compound was a D(2)A-type layered magnet, [{Ru-2(O2CPh-2,3,5-Cl-3)(4)}(2)(TCNQMe(2))]center dot 4DCM (1; 2,3,5-Cl3PhCO-2 = 2,3,5-trichlorobenzoate; TCNQMe(2) = 2,5-dimethyl-7,7,8,8-tetracyanoquinodimethane; DCM = dichloromethane), where [Ru-2(O2CPh-2,3,5-Cl-3)(4)] ([Ru-2(II,II)) is an electron donor (D) and TCNQMe(2) is an electron acceptor (A). Compound 1 had a one-electron-transferred, charge-ordered state with a [{Ru-2(II,II)}-TCNQMe(2)(center dot-){Ru-2(II,III)}(+) ](1e-I) formula. Strong intralayer antiferromagnetic couplings between [Ru-2(II,II)} with S = 1 or [Ru-2(II,III)](+) with S = 3/2 and TCNQMe(2)(center dot-) with S = 1/2, as well as ferromagnetic interlayer interactions, induced long-range ferrimagnetic ordering at T-c = 101 K. Interstitial DCM molecules were located between layers, and these were gradually eliminated under vacuum at 80 degrees C to form a solvent-free compound (1-dry) without loss of crystallinity. The electronic state of 1-dry thermally fluctuated and eventually provided a charge-disproportionate disordered state, with a [{Ru-2}(0.5+)-TCNQMe(2)(1.5)-{Ru-2(II,III)}(+)] (1.5e-I) formula as the ground state. The T-c in 1-dry was 34 K because of the presence of diamagnetic TCNQMe(2)(2-) in some parts of the framework. A large T-c variation with Delta T-c R approximate to 70 K was switchable; switching was achieved by charge-state modulations accompanied by subtle structural modifications in solvation/desolvation treatments.