Dielectric constant, resistivity, and dissipation factors at 100 Hz to 1 MHz are reported for three zirconium phosphate/phosphonate-based self-assembled multilayers: Zr biphenylene-diphosphonate, a polar azo dye multilayer, and Zr pyrophosphate, all deposited on gold. Experiments with mercury drop top electrodes indicate that these materials are good insulators, with dielectric constants of 3-6 when dry. The magnitudes and frequency dependences of the constants are greatly altered when the layers are hydrated. While the dielectric strength of the materials is sufficient for applications including electrooptics, the porosity of the films to water and evaporated metals needs to be reduced before practical use may be considered.