Phosphors with a longer excitation wavelength exhibit higher energy conversion efficiency. Herein, quantum cutting KGd(CO3)2:Tb3+ phosphors excited by middle-wave ultraviolet were synthesized via a hydrothermal method. All the KGd(CO3)2:xTb3+ phosphors remain in monoclinic structures in a large Tb3+ doping range. In the KGd(CO3)2 host, 6D3/2 and 6I17/2 of Gd3+ were employed for quantum cutting in sensitizing levels. The excited state electrons could easily transfer from Gd3+ to Tb3+ with high efficiency. There are three efficient excited bands for quantum cutting. The excited wavelengths of 244, 273, and 283 nm correspond to the transition processes of 8S7/2→6D3/2 (Gd3+), 8S7/2→6I17/2 (Gd3+), and 7F6→5F4 (Tb3+), and the maximum quantum yields of KGd(CO3)2:Tb3+ can reach 163.5, 119, and 143%, respectively. The continuous and efficient excitation band of 273–283 nm can well match the commercial 275 nm LED chip to expand the usage of solid-state light sources. Meanwhile, the phosphor also shows good excitation efficiency at 365 nm in a high Tb3+ doping concentration. Therefore, KGd(CO3)2:Tb3+ is an efficient green-emitting phosphor for ultraviolet-excited solid-state light sources.