Li2MgTiO4:Cr3+, Mn4+ phosphors were successfully synthesized by the high-temperature solid-state reaction method. Cr3+, Mn4+ co-doped Li2MgTiO4 phosphors have two emission peaks at 674 nm and 719 nm, corresponding to 2E→4A2 transitions of Mn4+ and 2E→4A2 transitions of Cr3+, respectively. The two emission peaks are matched with the absorption of PR and PFR, and the intensity ratio of the two emission peaks is adjusted by changing the doping concentration of Mn4+, indicating that the phosphors have potential applications in plant cultivation. In addition, it can be observed that the emission peak corresponding to Mn4+ can decrease sharply with the increase of excitation wavelength, while the emission peak corresponding to Cr3+ can change little, which indicates that the phosphors can be used for wavelength detection. The security ink prepared by Li2MgTiO4:Cr3+, Mn4+ phosphors shows that it can be applied in anti-counterfeiting labels. These results suggest that Li2MgTiO4:Cr3+, Mn4+ have the great potentiality to be used for plant cultivation, wavelength detection and anti-counterfeiting.