By introducing Ti vacancies for valence compensation, Nd-doped SrTiO3 ceramics yielding the formula NdxSr1-xTi1-x/4O3 (0≤x≤0.200) were successfully prepared by solid state reaction route in air. All the ceramics had single perovskite structure indexed by XRD profiles, while the symmetry changed from cubic to tetragonal with increasing x value. The grain size markedly decreased from ~30 μm for un-doped SrTiO3 ceramics to ~1 μm for NdxSr1-xTi1-x/4O3 ceramics with x=0.024, which was observed by scanning electron microscopy (SEM). The dielectric properties were measured at 1 kHz in ambient temperature. The dielectric constant was found to be leading to a maximum value of 5410 for as-sintered sample with x=0.104. The breakdown strength of all NdxSr1-xTi1-x/4O3 samples was examined to be higher than 10 kV/mm. These results indicated that Nd-doped SrTiO3 ceramics could be used to fabricate high voltage capacitors with enhanced energy storage density.