Tb3+ is a typical green-emitting activator and in some cases could sensitize Eu3+ through energy transfer, leading to color tunable emissions by changing their relative contents. In this work, Tb3+ and Tb3+/Eu3+ were singly- and co-doped into the borate host LiSrY2(BO3)3 with the formulas LiSr(Y1-xTbx)2(BO3)3 (0 <x ≤ 1) and LiSr(Y0.7-yTb0.3Euy)2(BO3)3 (0.001 ≤ y ≤ 0.03). Powder XRD confirms the phase purity by extracting the cell lattice parameters, which exhibit a linear dependence on doping contents. Due to the local symmetry-broken characteristic of the rare earth cation in this host, relatively strong f-f excitations in the NUV range were observed for Tb3+-phosphors, and concentration quenching effect was observed at x = 0.30 and 0.50 when excited by 260 and 365 nm, respectively. As expected, the Tb3+ to Eu3+ energy transfer was confirmed, thus was utilized to color tunable emissions from green to red.