Vinyl ester matrix syntactic foams filled with hollow glass microballoons (GMBs) are investigated for the possibility of simultaneously tuning their electrical, thermal and mechanical properties. Six different compositions have been investigated to develop a relation between the dielectric constant and hollow particle parameters such as volume fraction and radius ratio. The dielectric constant of syntactic foams decreased with increase in volume fraction and increased with increase in the radius ratio of MBs. To further elucidate the effect of volume fraction and radius ratio on the dielectric constant, a parametric study has been performed based on a theoretical model developed for syntactic foams. This study suggested that several compositions of syntactic foams can be developed to obtain same dielectric constant but different coefficient of thermal expansion, elastic modulus and density. These results provide a unique approach of tailoring the dielectric constant independent of the density or other mechanical and thermal properties of syntactic foams. Simultaneous tailoring of two or more properties of syntactic foams can help in developing multifunctional materials.