The past decade has witnessed a substantial increase in research on synthesis techniques for pure and dopedcarbon nanotubes and their involved parameters. However, there is a missing link between the ideal synthesisconditions for high quality functionalized structures with heteroatoms such as nitrogen and the formation ofdifferent bonding environments through the actual process. We describe here an approach to prepare highquality and substitutionally N-doped single and double walled carbon nanotubes with a defined diameterrange from a nondiluted carbon/nitrogen feedstock. This not only illustrates the dependence on the combinedsynthesis parameters but also provides a fundamental insight into the formation of nitrogen volatile speciesduring the feedstock pyrolysis versus the actual N-incorporation profile within the walls.