This report focuses on the comparison of the effects of two different halogen dopants (bromine and iodine) on the Raman spectra of “double-walled carbon nanotube (DWNT) buckypaper”. By changing the laser excitation energy, it is possible to study the effects of the dopants on different DWNTs. We observed that the Raman spectra of these doped DWNTs are dominated by the stretching bands of the dopants. The frequency of both the ωBr−Br and ωI−I bands showed a dependence on the laser excitation energy. Specifically, a minimum of the frequency of the halogen-based bands occurred when the halogen species were in electronic resonance with Elaser. This can be explained by the stronger interaction between dopant molecules and the carbon molecules in the DWNTs when the electronic resonance is at a maximum.