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The complete transformation from narrow peak emission of Eu 3+ to broadband emission of Eu 2+ was first realized in La 1- x Sr 2+ x Al 1- x Si x O 5 :Eu series solutions relying on crystal field engineering and adjustment of synthesis parameters. The original red phosphor La 0.97 Sr 2 AlO 5 :0.03Eu 3+ peaks at 703 nm originated from 5 D 0 → 7 F 4 transition of Eu 3+ under 395 nm excitation. As the x value regularly increased, Sr 2 SiO 4 -type green phosphor La 0.17 Sr 2.8 Al 0.2 Si 0.8 O 5 :0.03Eu 2+ was synthesized at x = 0.8, which can be efficiently excited by UV/blue light chips. Moreover, when x > 0.975, Sr 3 SiO 5 :Eu 2+ type broadband orange phosphor Sr 2.945 Al 0.025 Si 0.975 O 5 :0.03Eu 2+ with excellent thermal stability (91.3% peak intensity at 150 °C) was obtained. Variations in the crystal structure, phase, and luminescence properties were studied in detail. We hope this work can provide a reference that solid solution between distinct but structurally related systems is a strategy to explore the possible phosphors for phosphor-converted light-emitting diodes.