C70 nanotubes with a fcc lattice structure are polymerized through being irradiated by lasers with a wavelength of 514.5 nm at various power values. Raman spectra and photoluminescence (PL) spectra are employed to characterize the polymeric phases of the laser treated samples, showing that the disordered C70 oligomers are formed in the C70 nanotubes irradiated by such strong green lasers. Comparative studies further indicate that intermolecular bonds are formed between C70 molecules on the surface of nanotubes, which are similar to those formed under high pressure and high temperature (HPHT) conditions. And the content of intermolecular bonds increases obviously with the laser power increasing.