Floating catalyst chemical vapor deposition (FCCVD) enables ultrafast synthesis of CNTs and other 1D nanoparticles and their direct assembly as macroscopic solids. The chalcogen growth promotor in FCCVD produces high aspect ratio CNTs that can aggregate in the gas phase and form an aerogel which can be continuously spun as macroscopic fibres or sheets. We study the role of sulphur in controlling CNT morphology and aggregation by synthesising CNTs under a wide range of S/C ratios (0.001 to 5 wt.%) and determining their diameter and length distributions, number concentration and form of aggregation. Increasing S/C ratio in this range increases mean number of CNT walls from 1 to 8, decreases mean length from 34 to 6 µm, but CNT number concentration remains approximately constant at 8 × 108#/cm3. Assuming growth within the first 3 cm of the reactor, longitudinal growth rate spans 1.5- 6.5 µm/s for the different CNT morphologies, but with similar mass throughput of 700 attogram/catalyst. This indicates the amount of carbon reaching the catalyst and solidifying as CNT remains constant regardless of the sulphur available in the catalyst, suggesting the rate limiting process is not at the catalyst/promoter interface but instead in the transport of carbonaceous active precursors to the catalyst, either due to their diffusion in the gas phase or decomposition kinetics. The CNTs produced range from polymer-like, which readily bundle and form aerogels, to rod-like that do not. We include aerogelation “phase diagrams” for different CNT concentrations, aspect ratios and CNT bending stiffness.