We report in this paper the preparation and magnetic properties of layered metal(II) hydroxynitrates and hydroxyacetates which display, according to the metal ion, either ferro (Co(II) and Ni(II)) or antiferromagnetic (Cu(II)) intralayer interactions. These compounds are shown to be suitable host lattices for organic species. 2,6- and 2,5- pyridine-based nitronyl-nitroxide biradicals have been synthesized and their magnetic properties investigated. They respectively display ferro- and antiferromagnetic behaviors. X-rays studies show an angle of 88 degrees (in the 2,6 case) and 0 degrees (in the 2,5 case) between both radicals. The synthesis of a new imino-nitroxide benzoic acid radical characterized by classical methods and X-rays diffraction, and preliminary results of exchange reaction with copper(II) basic salts are also discussed.