E-1-(1″-hydroxycarbonylferrocen-1′-yl)-2-(cycloheptatrienyl)ethene (4) was synthesized by using selective transmetallation reactions. Reaction of 4 with [Cp*Ru(CH 3 CN) 3 ](PF 6 ) revealed the vinylogue monohydro sesquifulvalene complex E-1-(1″-hydroxycarbonylferrocen-1′-yl)-2-{(1‴-6‴-η-cyclohepta-1‴,3‴,5‴-trien-1‴-yl)(η 5 -pentamethylcyclopentadienyl)ruthenium(II)}ethene hexafluorophosphate (5). X-ray structure analysis demonstrates that complex 5 crystallizes in the triclinic space group P1¯, which forms discrete dimers via two hydrogen bonds between the carboxylic functions. Reaction of complex 5 with triethylamine or NaHCO 3 generated a new organometallic zwitterion E-1-(1″-oxycarbonylferrocen-1′-yl)-2-{(1‴-6‴-η-cyclohepta-1‴,3‴,5‴-trien-1‴-yl)(η 5 -pentamethylcyclopentadienyl)ruthenium(II)}ethene (6), which was characterized by UV, IR, and NMR spectra.