We report here investigations on the superstructure modulation induced by the ordering of carbon vacancies in the nonstoichiometric zirconium carbide of ZrC0.61, which was prepared by spark plasma sintering (SPS) of the mechanochemically synthesized ZrCx nanopowders. The sintered ZrC0.61 is found to exhibit an interesting microstructure of interlaced laminated sheets. In contrast to the previous long duration post annealing for realization of the ordered carbon vacancies in the rocksalt-structured transition metal carbide, the ordered carbon vacancies are directly obtained during the SPS process, and no post-annealing period is necessary. With the help of transmission electron microscopy, the superstructural nanodomains with the average size of ∼30 nm are identified.