Carbon nanotubes come in many varieties, with chemical, mechanical, and electrical properties depending on carbon nanotube (CNT) structural morphology. In order to provide a platform for CNT structural tuning, a membrane reactor was designed and constructed. This reactor provided more intimate gas-catalyst contact by decoupling the carbon feedstock gas from carrier gas in a chemical vapour deposition (CVD) environment using an asymmetric membrane and a macroporous membrane. Growth using this membrane reactor demonstrated normalized yield improvements of ∼300% and ∼1000% for the asymmetric and macroporous membrane cases, respectively, over standard CVD methods. To illustrate the possibility for control, growth variation with time was successfully demonstrated by growing vertically aligned multi-walled CNTs to heights of 0.71 mm, 1.36 mm, and 1.84 mm after growth for 15, 30, and 60 minutes in a commercial thermal CVD reactor. To demonstrate CNT diameter control via catalyst particle size, dip coating and spray coating methods were explored using ferrofluid and Fe(NO3)3 systems. CNT diameter was demonstrated to increase with increasing particle size, yielding CNT like growth with diameters ranging from 15 -150 nm. Demonstration of these dimensions of control coupled with the dramatic efficiency increases over growth in a commercialized CVD reactor establish this new reactor technology as a starting point for further research into CNT structural tuning.