Incorporation of indium (dopant) into CdS crystals have been successfully achieved by a mechanical alloying process. Powders are prepared with various In/Cd ratio from 1 to 10 at% and milled at 300 revolution per minute (rpm) for 60 min. X-ray diffraction (XRD) analysis of milled In doped CdS compound showed that the major phase of the product was wurtzite with grain sizes varying from 37 to 42 nm corresponding to change in In/Cd compositions. High resolution transmission electron microscopy (HRTEM) images as well as Fourier transformation in reciprocal space provide a good pathway to identify the structure of individual CdS nanocrystals, whose dominant phase was determined to be wurtzite structure along with zinc blende structure. Field emission scanning electron microscopy (FESEM) images reveal that CdS crystal prefers to grow along the (001) direction rather than (110) due to its high surface energy. The Raman spectra of CdS:In particles present well-resolved lines at approximately 303 and 600 cm(-1), corresponding to the first and second-order scatterings, respectively, of the longitudinal optical (LO) phonon mode. Dielectrical studies showed that dielectrical constant (epsilon') decreased with increase in frequency, whereas AC conductivity (sigma(AC)) in In doped CdS increases with increase in frequency and also both the values increased with increase in doping concentration.