Composition-tunable ternary CdxPb1−xS nanocrystals (NCs) are very important materials for remote sensing and detecting in the infrared (IR) wavelength region. They are, however, almost exclusively prepared by wet chemical routes which lead to surface-capped nanoparticles. The surface capping molecules could move their absorption peaks from mid-IR to near IR wavelength region. However, surface clean CdxPb1−xS nanocrystals (NCs) would demonstrate intrinsic optical spectrum in the mid-IR region. Herein, we present a physical mechanical alloying (MA) process being applied to prepare tens of grams of surface clean CdxPb1−xS nanocrystals within the composition range of x = 0.0 to 0.4. The average particle size is smaller than 9 nm. The as-milled nanocrystals are chemically homogenous. The CdxPb1−xS nanocrystals show a continuous lattice contraction with Cd content. There is an exponential indirect band gap-composition relationship. This MA method shows the ability to continuously and precisely tune the band gap energies of ternary CdxPb1−xS semiconductor nanocrystals from mid-IR region (2638 nm) to NIR wavelength region (1240 nm) through chemical composition.