Six new zinc phosphite hybrids are prepared under a variety of reaction conditions from the primary building blocks, trimethylenedipyridine, zinc acetate, and phosphorous acid. Neutral guest molecules are incorporated into several of the structures. Under hydrothermal conditions at 130 degrees C, an anionic framework structure, 1, templated on trimethylenedipyridinium, is obtained while a neutral ladder structure, 2, is formed at room temperature. These reactions are done at an initial pH of 4.7-5.0. When the reaction is done at an initial pH of 7.8-8.0, a neutral layered motif is obtained with 1,3-dipyridylpropane pillars and neutral guests in the interstitial space. Structures with water, phenol, and catechol as the guests, compounds 3, 4, and 5, respectively, are reported. The use of catechol as a template results in the breakup of the ZnPO sheet structure common to both 3 and 4. When amino acids, including alanine, were added to the reaction medium, a neutral three-dimensional framework, 6, is obtained with no incorporation of the potential template. The syntheses and structures of these new materials are reported.