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Robust electrode materials without the addition of binders allow increasing efficiency of electrical storage devices. We demonstrate the fabrication of binder-free electrodes from modified single-walled carbon nanotubes (SWCNTs) for electrochemical double-layer capacitors (EDLCs). Modification of SWCNTs included a sonication in 1,2-dichlorobenzene and/or fluorination with gaseous BrF3 at room temperature. The sonication caused the shortening of SWCNTs and the splitting of their bundles. As a result, the film prepared from such SWCNTs had a higher density and attached a larger amount of fluorine as compared to the film from non-sonicated SWCNTs. In EDLCs with 1M H2SO4 electrolyte, the fluorinated films were gradually defluorinated, which lead to an increase of the specific capacitance by 2.5–4 times in comparison with the initial values. Although the highest gravimetric capacitance (29 F g−1 at 100 mV s−1) was observed for the binder-free film from non-modified SWCNT, the fluorinated film from the sonicated SWCNTs had an enhanced volumetric capacitance (44 F cm−3 at 100 mV s−1). Initial SWCNT films and defluorinated films showed stable work in EDLCs during several thousand cycles.