In this study, we successfully synthesize cationic/neutral/anionic inverse-Hofmann-type spin crossover (SCO) frameworks with 1,1,2,2-tetrakis(4-(pyridine-4-yl)phenyl)-ethene ligand by means of cyanometallic charge engineering strategy. The cationic and neutral frameworks exhibit single-step thermally induced spin transition behaviors, while the SCO capability of anionic framework can be aroused by partial desolvation. This strategy provides a new idea to construct ionic SCO frameworks and extends the toolkit for SCO materials.