Lead sulfide ( PbS ) nanocrystals anchored on nitrogen-doped multiwalled carbon nanotubes ( CNx ) have been synthesized employing an environmentally friendly and inexpensive wet chemistry process. CNx∕PbS composites have been examined by scanning electron microscopy, X-ray diffraction and Raman spectroscopy. Theorical ab initio calculations have been developed to determine the samples structural, morphological and optical properties to explain the experimental evidences. The PbS nanoparticles exhibit of 4 nm to 27 nm particle size with a face-centered cubic crystal structure and are homogeneously distributed along the carbon nanotubes. The nitrogen-doped CNTs acts as binding sites for the PbS clusters as ab initio theoretical study suggests.