A facile electrodeposition technique was utilized to deposit single-walled carbon nanotubes (SWNTs) with cadmium telluride (CdTe) with well-controlled size, density, surface morphology, and composition. By controlling the applied charge, the morphology of these hybrid nanostructures was altered from CdTe nanoparticles on SWNTs to SWNT/CdTe core/shell nanostructures and the composition of the CdTe nanoparticles was altered from Te-rich (29 at% Cd) to Cd-rich (79 at% Cd) CdTe by adjusting the deposition potential. The electrical and optoelectrical properties of these hybrid nanostructures showed that photo-induced current can be tuned by tailoring the conductivity type (n-type or p-type), morphology, and size of the CdTe nanostructures, with a maximum photosensitivity (ΔI/I(0)) of about 30% for SWNT/Cd-rich CdTe (n-type) core/shell nanostructures. This work demonstrates a novel approach for synthesizing metal chalcogenide/SWNT hybrid nanostructures for various electrical and optoelectrical applications.