To address challenges in enhancing color uniformity and ambient contrast ratio (ACR) in RGB light-emitting diodes (LEDs) without losing efficiency, we developed a scattering-enhanced magnetic manipulation (SEMM) bilayer structure. The effect of the TiO2 scattering layer on improving the LED’s angular intensity non-uniformity (AIN) was studied by ray-tracing simulations and optimized by varying the particle concentration. The magnetic manipulation technique formed the microcolumns and magnetic chains of the Fe3O4 anti-reflective layer, which was optimized by adjusting Fe3O4 particle size, magnetic field strength, and Fe3O4 concentration. The resulting bilayered device significantly increased the ACR by 11.38 times and reduced AIN by 63% compared to conventional graphite-based LEDs, while maintaining high brightness and consistent color quality across angles. This marks a pioneering application of magnetic manipulation in enhancing LED display quality.