The application of single-walled carbon nanotubes (SWCNTs) as saturable absorbers (SA) in a Nd:glass femtosecond laser is verified as a promising alternative to traditional semiconductor saturable-absorber mirrors (SESAMs). The shortest laser pulses achieved with a SWCNT-SA fabricated by the slow-evaporation method are reported herein. Nearly Fourier-limited 288 fs pulses are obtained with negative-dispersion soliton mode-locking. The importance of the properties of the starting material, such as the degree of purity and the chirality, and the successive slow-evaporation deposition method is proven by using a multitechnique approach based on X-ray diffractometry, scanning electron microscopy, and μ-Raman spectroscopy. The high degree of nanotube alignment on the glass substrate and also the slight metallic character due to electron transfer between the glass matrix and the nanotubes themselves are identified as the main features responsible for the good laser response.