In this work, we described a facile route for the fabrication of free-standing single-walled carbon nanotubes (SWCNT)-CdSe quantum dots (QDs) hybrid ultrathin films and investigated their optoelectronic conversion properties. A free-standing SWCNT film with thickness of ∼36 nm was firstly prepared via vacuum filtration. The film was then immersed into the pre-synthesized oleic acid-capped CdSe QDs (average diameter of 3.5 nm) solution, where CdSe QDs anchored spontaneously onto the surface of SWCNT film to produce SWCNT-CdSe QDs hybrid film. By using pure SWCNT films in different thicknesses as bottom and top electrodes, a flexible all-carbon electrode optoelectronic conversion device with sandwich structure of SWCNT film (thickness of ∼200 nm)/SWCNT-CdSe QDs hybrid film (thickness of ∼36 nm)/SWCNT film (thickness of ∼36 nm) was constructed to generate optoelectronic conversion under illumination of solar-simulated light. Our results demonstrated that the all-carbon electrode structure was effective for charge separation and a sensitive and stable photocurrent signal could be produced in such a device. In addition, our SWCNT-CdSe QDs hybrid film exhibited high flexibility and durability. No clear change in the resistance of the film was detected under bending in various bending angles.