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We have developed a versatile catalyst-assisted chemical vapor deposition (CVD) technique for the synthesis of single-walled carbon nanotubes (SWNTs) from discrete nickel nanoparticles (average diameter of 4.7 ± 1.5 nm). Atomic force microscopy (AFM), transmission electron microscopy (TEM) and electron diffraction are used to characterize these as-grown nanotubes. On a particular sample we found that the SWNTs have an average chiral angle of 25.3°. This result shows that a control of the chiral angle of SWNT with large diameters (mean diameter = 1.75 nm) and with a relatively broad diameter distribution (standard deviation = 0.5 nm) is achievable to a certain extent.