Sunlight-excitable orange or red persistent oxide phosphors with excellent performance are still in great need. Herein, an intense orange-red Sr3-xBaxSiO5:Eu(2+),Dy(3+) persistent luminescence phosphor was successfully developed by a two-step design strategy. The XRD patterns, photoluminescence excitation and emission spectra, and the thermoluminescence spectra were investigated in detail. By adding non-equivalent trivalent rare earth co-dopants to introduce foreign trapping centers, the persistent luminescence performance of Eu(2+) in Sr3SiO5 was significantly modified. The yellow persistent emission intensity of Eu(2+) was greatly enhanced by a factor of 4.5 in Sr3SiO5:Eu(2+),Nd(3+) compared with the previously reported Sr3SiO5:Eu(2+), Dy(3+). Furthermore, Sr ions were replaced with equivalent Ba to give Sr3-xBaxSiO5 :Eu(2+),Dy(3+) phosphor, which shows yellow-to-orange-red tunable persistent emissions from λ=570 to 591 nm as x is increased from 0 to 0.6. Additionally, the persistent emission intensity of Eu(2+) is significantly improved by a factor of 2.7 in Sr3-xBaxSiO5 :Eu(2+),Dy(3+) (x=0.2) compared with Sr3SiO5 :Eu(2+),Dy(3+). A possible mechanism for enhanced and tunable persistent luminescence behavior of Eu(2+) in Sr3-xBaxSiO5:Eu(2+),RE(3+) (RE=rare earth) is also proposed and discussed.