Near-infrared phosphor converted light-emitting diodes (NIR pc-LEDs), as a state-of-the-art type of NIR sources, are finding multifaceted applications, where phosphor is a crucial component. In hope to provide new choices for NIR lighting, we synthesized in this work the two series of Ruddlesden -Popper type layered perovskite phosphors of SrLa2Al2-xO7:xCr3+ (x = 0–0.02) and SrLa2-yGdyAl1.984O7:0.016Cr3+ (y = 0–2), followed by detailed structure and luminescence investigation. SrLa2Al2-xO7:xCr3+ was found to emit ∼700–800 nm NIR light under UV excitation and be able to maintain ∼54.3 % of its room temperature intensity at 423 K, which is remarkably higher than those (∼25–30 %@423 K) of the Mn4+ activated perovskite NIR phosphors. Luminescence regulation was achieved by substituting La3+ with Gd3+, and it was revealed that Gd3+ may act as a sensitizer to significantly enhance Cr3+ luminescence (∼346 % at 77 K) through Gd3+ → Cr3+ energy transfer, which was confirmed by spectral and fluorescence lifetime analysis. The observed spectral features and the influence of Gd3+ were rationalized by considering crystal structure, local coordination, and crystal field. Finally, an NIR pc-LED device showing strong ∼700–900 nm luminescence was fabricated to show potential application of the phosphor in night vision and plant lighting.