Millimeter-tall vertically aligned single-walled carbon nanotubes (SWCNTs) were grown in 10-15 min by chemical vapor deposition from C(2)H(2)/Ar with or without water addition using Fe catalyst supported on an Al-Si-O underlayer. Using combinatorial catalyst libraries coupled with the real-time monitoring of SWCNT growth, the catalyst and chemical vapor deposition conditions were systematically examined, and millimeter-tall SWCNTs were obtained even without water addition. The key for millimeter-scale growth of SWCNTs is to limit the C(2)H(2) supply to below a certain partial pressure to retain an active catalyst. Water prolongs the catalyst lifetime under excess C(2)H(2) supply, whereas it deactivates small catalyst particles and degrades the quality of SWCNTs at the same time. We also observed a gradual increase in the diameter of SWCNTs with growth because of the coarsening of catalyst particles and found that water had no effect on this phenomenon. We demonstrate millimeter-tall SWCNTs grown by simply using C(2)H(2)/Ar gas without water addition, which revealed the mysterious role of water, and we show a practical route for the large-scale production of SWCNTs.