Silicon-vacancy (SiV) centers were produced in single crystalline diamond (SCD) and ultrananocrystalline diamond (UNCD) nanostructures via Si ion implantation or in situ Si doping. SiV-embedded UNCD (SiV-UNCD) was fabricated by both top-down and bottom-up methods. The spectral properties of the SiV centers, including the zero phonon line (ZPL) width and decay time, were investigated in the SCD and UNCD nanostructures. All the SiV-UNCD nanostructures showed bright emission regardless of the preparation method. However, the decay time of the SiV centers was affected by the synthesis procedure. A SiV decay time of τ ∼0.19 ns was observed for UNCD nanostructures formed by in situ doping, whereas the SiV decay time was ∼0.43 ns for SiV-UNCD clusters prepared by Si ion implantation into UNCD deposited on Ti/sapphire substrates. The ultrasonication of UNCD clusters on Ti/sapphire pyramids produced bright SiV-UNCD nanoclusters with sizes of ∼50 nm, a ZPL width of 13.5 nm, and a decay time of 0.35 ns, suggesting promising potential in bioimaging applications. SiV-containing SCD (type Ia or type IIa) showed enhanced SiV spectral properties with a ZPL width of 6.08 nm and longer decay time of 1.3 ns.