A series of new metal organic frameworks, namely, [Ag(mapym)(suc)(0.5)center dot 0.5H(2)O](n) (1), [Ag-2(mapym)2(glu)center dot 1.5H(2)O] (2), [Ag-2(mapym)(2)(ipa)center dot 2H(2)O](n) (3), [Ag-2(mapym)(2)(tpa)(H2O)](n) (4), [Ag(dmapym)(2)(ox)(0.5)center dot H2O] (5), and [Ag(dmapym)(bbdc)(0.5)center dot 0.5H(2)O](n) (6) (mapym = 2-amino-4-methylpyrimidine, dmapym = 2-amino-4,6-dimethylpyrimidine, H(2)suc = succinic acid, H(2)glu = glutaric acid, H(2)ipa = isophthalic acid, H(2)tpa = terephthalic acid, H(2)ox = oxalic acid, H(2)bbdc = 4,4-bibenzenedicarboxylic acid), have been synthesized and structurally characterized. Complexes 1 and 2 exhibit two-dimensional (2D) interpenetrated and double-sheet structures, respectively. Complex 3 is a three-dimensional (3D) framework constructed through unusual 2D -> 3D parallel interpenetration of a corrugated 2D 4(4)-sql net. Complex 5 is a 0-dimensional (0D) H-shaped molecule, and the self-complementary N-H center dot center dot center dot N hydrogen bonds incorporating R-4(4)(14) hydrogen bond motifs extend these molecules into a 3D supramolecular framework. Complexes 4 and 6 are also 2D sheets constructed with a similar fashion to that of 1 and 2 but with aryl-dicarboxylate as bridge. The results show that the coordination geometry of the Ag(I) ions and the configuration and coordination mode of dicarboxylates as well as the competition between steric and electronic effects of methyl groups on aminopyrimidyl ligands play crucial roles in determining the structure of the complexes. Additionally, results about IR spectra, thermogravimetric curves, and photoluminescence spectra were addressed.