This present article investigates the influence of doping Sm3+ ions in the Ba3Zr2O7 host lattice. The solution combustion route is employed to prepare a series of Ba3(1-x)Zr2Sm3xO7 (x = 0.005, 0.01, 0.015, 0.02, 0.025, and 0.03) samples. The structural studies are carried out by X-ray diffraction (XRD) technique and the phosphor exhibits a tetragonal phase. The chemical compositions and oxidation state of the elements present on the surface of the phosphor are investigated using the XPS technique. PL emission spectra yield four emission bands amongst them a strong emission band is observed at wavelength 602 nm imparting orange-red color owing to the electronic transition 4G5/2→6H7/2 of Sm3+ ion. The impact of doping of Sm3+ ions on the phosphor’s luminescence spectra has been prominently featured. The optical parameters such as energy band gap, metallization criterion, and refractive index, for the optimal molar concentration (1.5 mol%) are 4.92 eV, 0.49, and 1.74, respectively. Based on these findings, the Sm3+ -activated Ba3Zr2O7 phosphor appears to be an excellent candidate for filling the amber gap in LEDs.