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Mn-based phosphors with the wavelength of 700–750 nm are an important category of far-red phosphors that have promising potential in the application of plant lighting, and the higher ability of the far-red light emitting of the phosphors is beneficial to plant growth. Herein, a series of Mn4+- and Mn4+/Ca2+-doped double perovskite SrGd2Al2O7 red-emitting phosphors with wavelengths centered at about 709 nm were successfully synthesized by means of a traditional high-temperature solid-state method. First-principles calculations were conducted to explore the intrinsic electronic structure of SrGd2Al2O7 for a better understanding of the luminescence behavior in this material. Extensive analysis demonstrates that the introduction of Ca2+ ions into the SrGd2Al2O7:Mn4+ phosphor has significantly boosted the emission intensity, internal quantum efficiency, and thermal stability by 170%, 173.4%, and 113.7%, respectively, which are superior to those of most other Mn4+-based far-red phosphors. The mechanism of the concentration quench effect and the positive effect of co-doping Ca2+ ions in the phosphor were extensively explored. All studies suggest that the SrGd2Al2O7:0.1%Mn4+, 11%Ca2+ phosphor is a novel phosphor that can be used to effectively promote the growth of plants and regulate the flowering cycle. Therefore, promising applications can be anticipated from this new phosphor. [ABSTRACT FROM AUTHOR]