Silver(I) complexes of two designed tridentate ligands, namely, 2, 6-(pyridyl)-iminoditriazaadamantane (pydTAm) and 2,6-(pyridyl)-iminodiadamantane (pydAm), have been synthesized and structurally characterized. [Ag(pydTAm)(2)](CF3SO3) (1), the hitherto unknown mer isomer of a silver(I) octahedral complex, crystallizes in a highly symmetric body-centered cubic I (4) over bar 3m space group. Quite in contrast, the Ag-I center in the analogous [Ag(pydAm)(2)](CF3SO3) (2) complex resides in a trigonal-bipyramidal geometry and crystallizes in a triclinic P (1) over bar space group with two crystallographically independent molecules in the asymmetric unit. Complex 1 exhibits exceptional solubility in aqueous media and leads to the efficient eradication of several bacterial strains upon sustained release of bioactive silver.