The self-assembly of extended metal-containing arrays is described based on dynamic coordination chemistry at mercury(II) with bis(amidopyridyl) ligands to form macrocycles, polymers, or sheets which can be further organized by hydrogen bonding between amide substituents. The ligands 1,2-C6H4{NHC(O)-4-C5H4N}(2), 1, 1,2-C6H4{C(O)-NHCH2-4-C5H4N}(2), 2, and 1,2-C6H4{CH2C(O)NHCH2-4-C5H4N}(2), 3 can adopt polar conformations and so can confer helicity in their complexes. Several macrocycles of formula [(HgX2)(2)(mu-LL)(2)] (LL = 1, 2), with tetrahedral mercury(II) centers, were prepared in which individual molecules are further self-assembled via hydrogen bonding in the solid state to form one- or two-dimensional polymers or sheets. In one case, a one-dimensional polymer [{(HgX2)(mu-3)}(n)] was formed. It is shown that the mercury(II) centers can be six-coordinate in forming the sheet structure [{(HgX2)(mu-2)(2)}(n)], in which there are particularly large pores.