An organometallic sandwich compound of terephthalic acid, namely, [(eta(5)-Cp)Fe-II{eta(6)center dot(1,4-C6H4(COOH)(2))}](+) (H(2)1(+)), is reported, along with X-ray single crystal structures of [H1 center dot H(2)1][PF6] and H1. [H(2)1 center dot H1][PF6] was reacted with the nitrate salts of Co-II and Ni-II to yield a series of three-dimensional (3D) metal-organometallic framework (MOMF) materials of the composition [M-3(1)(4)(mu-H2O)(2)(H2O)(2)][NO3](2)center dot xsolvent (M = Co-II (2), Ni-II (3); xsolvent = 4EtOH, or 2DMF center dot 2H(2)O). These framework structures were shown by single crystal and powder x-ray diffraction to be polymorphic, possessing identical 3D body-centered tetragonal network topologies, but differing in the manner by which the [CpFe](+) groups are arranged within the two-dimensional, square grid sheets of the 3D networks. alpha-2-EtOH, beta-2-EtOH, alpha-3-EtOH, beta-2-DMF, and beta-3-DMF were thermally desolvated, giving rise to isolable apohosts of composition [M-3(1)(4)(mu-H2O)(2)(H2O)(2)][NO3](2) (M = Co-II (2), Ni-II (3)) that were shown by PXRD to possess different, as yet unknown, crystal structures. The desolvated apohosts were studied with respect to their ability to selectively reabsorb water and/or alcohols. They show a modest preference for the absorption of water and short chain, linear alcohols (< C4), with modest selectivity for 1-PrOH.