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Organometallic oligoamides built from three to four ferrocene amino acid units (H-Fca-OH,1-amino-1'-ferrocene carboxylic acid) fold into hydrogen bonded secondary structures featuring eight-membered rings by cooperative hydrogen bonds. NMR studies and DFT calculations (CAM-B3LYP, LANL2DZ, IEFPCM (THF) reveal that the organometallic zigzag foldamer structures are highly resistant toward denaturation by hydrogen bond acceptors such as dimethyl sulfoxide and 2,4-lutidine. Replacing one ferrocene amino acid unit by the organic alpha-amino acid glycine at the C-terminal end (Fca goes to Gly) significantly destabilizes the secondary zigzag structure facilitating denaturation by DMSO. Highly stabilized ordered poly(Fca) architectures are very attractive for future applications of switchable hydrogen-bonded redox-active materials.