Wereport the synthesis of silicon-vacancy (SiV) incorporated spherical shaped ultrananocrystalline diamond (SiV-UNCD) particulates (size∼1 μm) with bright luminescence at 738 nm. For this purpose, different granular structured polycrystalline diamond films and particulates were synthesized by using three different kinds of growth plasma conditions on the three types of substrate materials in the microwave plasma enhancedCVDprocess. The grain size dependent photoluminescence properties of nitrogen vacancy (NV) and SiV color centers have been investigated for different granular structured diamond samples. The luminescence ofNVcenter and the associated phonon sidebands, which are usually observed in microcrystalline diamond and nanocrystalline diamond films, were effectively suppressed inUNCDfilms andUNCDparticulates. Micron sized SiV-UNCD particulates with bright SiV emission has been attained by transfer of SiV-UNCD clusters on sodalime glass fibers to inverted pyramidal cavities fabricated on Si substrates by the simple crushing of UNCD/soda-lime glass fibers in deionized water and ultrasonication. Such a plasma enhancedCVD process for synthesizing SiV-UNCD particulates with suppressedNVemission is simple and robust to attain the bright SiV-UNCD particulates to employ in practical applications.