In this paper, we have demonstrated that dense bulk nanostructured ceramics can be synthesized from micrometer‐sized powders by using an electrical field‐activated sintering process. A dense Pb(Mg1/3Nb2/3)O3‐PbTiO3 ceramic with grain sizes of 20–100 nm was obtained from the starting powder of 1 to 10 μm. Structural and property analysis confirmed that the entire specimen is composed of nano‐sized grains. The significant microstructural refining is attributed to a pulsed electric field‐induced thermo‐mechanical fatigue process, which in situ“shattered” the large particles into nano‐sized grains during sintering. An advantage of this technique over the previous ones is that it avoids the usage of ultrafine nanometer‐sized powders, which are difficult to process and mass produce in an economic and consistent way. In principle, the process demonstrated here can be applied to other material systems.