A novel strategy for the fabrication of multiwall carbon nanotube-nanocrystal heterostructures is shown. Different quantum dots (QDs) with narrow size distributions were covalently coupled to carbon nanotubes (CNTs) and silica-coated CNTs in a simple, uniform, and controllable manner. The structural and optical properties of CNT/QD heterostructures are characterized by electron microscopy and photoluminescence spectroscopy. Complete quenching of the PL bands in both QD core and core/shell heterostructures was observed after adsorption to the CNTs, presumably through either carrier ionization or energy transfer. The deposition of a silica shell around the CNTs preserves the fluorescence properties by insulating the QD from the surface of the CNT.