Carbon nanotubes (CNTs) have attracted much interest because of their superior electrical, thermal, and mechanical properties. These unique properties of CNTs have come to the attention of many scientists and engineers worldwide, eager to incorporate these novel materials into composites and electronic devices. However, before the utilization of these materials becomes mainstream, it is necessary to develop protocols for tailoring the material properties, so that composites and devices can be engineered to given specifications. In this chapter, we review our recent studies, in which we investigate the nominal tensile strength and strength distribution of multi-walled CNTs (MWCNTs) synthesized by the catalytic chemical vapor deposition (CVD) method, followed by a series of high-temperature annealing steps that culminate with annealing at 2900°C. The structural-mechanical relationships of such MWCNTs are investigated through tensile-loading experiments with individual MWCNTs, Weibull-Poisson statistics, transmission electron microscope (TEM) observation, and Raman spectroscopy analysis.