Carbon nanotubes (CNTs) can be considered as semi-rigid all-carbon polymers. However, unlike conventional polymers that can form 3D networks such as hydrogels or elastomers through crosslinking with each other in solution, the cylindrical carbon lattice of CNTs was not believed to be directly crosslinkable in solution until our recent discovery of UV-defluorination driven direct CNT crosslinking. In this study, we further reveal that the UV-defluorination-driven crosslinked CNTs are metastable and can decompose more readily than fluorinated or pristine CNTs upon exposure to Raman laser irradiation. Specifically, we investigate the stability of UV-defluorinated single-walled and multi-walled fluoro-nanotubes using Raman spectroscopy under controlled varying laser power. The results indicate that both the defluorinated single-walled and multi-walled CNTs are thermally less stable than pristine CNTs or untreated fluorinated CNTs, which can be attributed to the strains on the crosslinking bonds created from the curved carbon lattice of linked CNTs. This instability, particularly evident under high-power laser irradiation, leads to combustion processes ignited at relatively lower temperatures that cause an extended burned area centered on the laser spot, offering potential future applications as mechanically robust, lightweight materials with feasible post-use degradation options.