Realizing a high color rendering index (CRI) in Ce:LuAG transparent ceramics (TCs) with desired thermal stability is essential to their applications in white LEDs/LDs as color converters. In this study, based on the scheme of configuring the red component by Cr3+ doping, an efficient spectral regulation was realized in Ce,Cr:LuAG TCs. A unilateral shift could be observed in both PL and PLE spectra. By constructing TC-based white LED/LD devices in a remote excitation mode, luminescence properties of Ce,Cr:LuAG TCs were systematically investigated. The CRI values of Ce:LuAG TC based white LEDs could be increased by a magnitude of 46.2%. Particularly, by combining Ce,Cr:LuAG TCs with a 0.5 at.% Ce:YAG TC, a surprising CRI values of 88 and 85.5 were obtained in TC based white LEDs and LDs, respectively. Therefore, Ce,Cr:LuAG TC is a highly promising color convertor for high-power white LEDs/LDs applied in general lighting and displaying.