This research focused on the nanosecond (Nd: YAG-1064 nm) laser pulse effect on the optical and morphological properties of chemically modified multi-walled carbon nanotubes (MWCNT). Two suspensions of MWCNT in tetrahydrofuran (THF) were prepared, one was submitted to laser pulses for 10 min while the other (blank) was only mechanically homogenized during the same time. Following the laser irradiation, the suspension acquired a yellow-amber color, in contrast to the black translucent appearance of the blank. UV-vis spectroscopy confirmed this observation, showing the blank a higher absorption. Additionally, photoluminescence measurements exhibited a broad blue-green emission band both in the blank and irradiated suspension when excited at 369 nm, showing the blank a lower intensity. However, a modification in the excitation wavelength produced a violet to green tuning in the irradiated suspension, which did not occur in the blank. Lastly, the electron microscopy analysis of the treated nanotubes showed the abundant formation of amorphous carbon, nanocages, and nanotube unzipping, exhibiting the intense surface modification produced by the laser pulse. Nanotube surface modification and the coexistence with the new carbon nanostructures were considered as the conductive conditions for optical properties modification.