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Eu2 -activated reddish-orange-emitting Ca3Si2O7 phosphors were synthesized with the addition of NH4Cl flux. When the phosphors were synthesized in a nominal composition of (Ca0.99Eu0.01)3Si2O7 without flux addition, a Ca3Si2O7 phase responsible for reddish-orange emission was identified to coexist with an intermediate phase of a-Ca2SiO4 for green emission. With the addition of NH4Cl flux, a-Ca2SiO4 was suppressed while the pure phase Ca3Si2O7 was obtained as the flux content was 3 wt%. Through varying the amount of flux, the emission color of samples can be tuned from green to reddish-orange, corresponding to the phase transformation from a-Ca2SiO4 to Ca3Si2O7. Through optimizing the doping concentration of Eu2 , the optimized photoluminescence (PL) properties for reddish-orange emission can be achieved, which makes this kind of phosphor prospective in the applications of the phosphor-converted white light emitting diodes (PC-WLEDs).