This work reports a high-density graphene/sulfur assembly for compact Li-S batteries with high volumetric capacity, which retains good structural stability and conductivity. This dense assembly was prepared by a reduction-triggered self-assembly of graphene oxide with simultaneous deposition of sulfur, followed by unique evaporation-induced spatial volume shrinkage. This assembly has an ultrahigh density, delivering an unprecedented volumetric capacity that is much higher than common carbon/sulfur cathodes. In particular, the unique spatial confinement derived from the shrinkage of the graphene/sulfur assembly is favorable for stabilizing sulfur cathodes.