Two general goals in multilayer ceramic capacitors (MLCC) have been the replacement of noble metal electrodes and avoidance of regulated and/or toxic materials. The former relates primarily to material cost while the latter relates to engineering, health, and environmental costs. Ideally, one would reach these goals with improved performance, i.e., accompanied by an increase in relative permittivity, material breakdown strength and resistivity, with a simultaneous decrease in dielectric loss and the temperature coefficient of permittivity. Attainment of the goals and desired performance clearly requires something other than an evolutionary approach. This work explores the efficacy of dipole-like substitutional pairs in achieving improved performance in a non-lead dielectric material. Specifically, dipole-like substituted ceramic BaTiO3, Ba[(M0.05Ta0.05)Ti0.9]O3 with M = Sc, Cr, Mn, or Fe, and more complex electric-field interaction ceramics, e.g., Ba[(M0.0333Ta0.0666)Ti0.9]O3 with M = Mn, Ni, or Cu, are being investigated as potential candidate materials for MLCC technology. Here, we report the temperature dependent (from room temperature to 900°C) electrical properties, relative permittivity, dissipation factor, and resistivity of Ba[(M0.05Ta0.05)Ti0.9]O3 with M = Sc, Cr, Mn, or Fe and Ba[(M0.0333Ta0.0666)Ti0.9]O3 with M = Mn, Ni, or Cu.