A multiwalled carbon nanotube (MWCNT) film surface was irradiated with a single pulse from a neodymium-doped yttrium aluminum garnet (Nd:YAG) laser. When an MWCNT film is irradiated with a pulsed Nd:YAG laser of 23.7 mJ/cm2, the calculated maximum surface temperature becomes 304 °C. The surface temperature increases from 595 to 2968 °C with an increase in laser power from 59.4 to 469 mJ/cm2. The MWCNT film is examined by increasing the intensity of the two characteristic Raman shifts ID (defect-induced mode: D-band) and IG (graphite-induced mode: G-band) to clarify the effect of pulsed Nd:YAG laser heating. Moreover, a new original image analytical method is developed to characterize CNTs from scanning electron microscopy (SEM) images. This method is useful for measuring the diameter of as-grown CNTs and those after annealing with a pulsed Nd:YAG laser. The number of detected diameters between 40 and 60 nm increases with an increase in laser energy density from 181 to 268 mJ/cm2.