Macroscopic carbon nanotubes (CNTs) with uniform structures are in great demand for use in composites and environmental materials. Here we demonstrate the controlled synthesis of spongy CNT blocks with isotropic properties and flexible, freestanding structures. The formation mechanism of the isotropic CNT sponges is discussed, based on its open-ended structure and initial formation in the vapor phase. The microstructure of the CNT sponges can be tuned by changing the flow rate of the carrier gas, resulting in CNT sponges with diameters ranging from 30.2 to 47.8 nm and wall thicknesses from 7 to 16 nm. The bulk density (5-25 mg cm), mechanical strength of the CNT sponges, and filling rate of ferromagnetic catalyst in the CNT sponges can also be modulated by controlling the supply rate of the carbon source, suggesting potential applications in mechanical energy absorption and environmental materials. © 2013 IOP Publishing Ltd.