The electrical and optical improvements of AlGaInP micro-light-emitting diodes (µLEDs) using atomic-layer deposition (ALD) sidewall passivation were demonstrated. Due to the high surface recombination velocity and minority carrier diffusion length of the AlGaInP material system, devices without sidewall passivation suffered from high leakage and severe drop in external quantum efficiency (EQE). By employing ALD sidewall treatments, the 20×20 µm2 µLEDs resulted in greater light output power, size-independent leakage current density, and lower ideality factor. The forward current-voltage characteristic was enhanced by using surface pretreatment. Furthermore, ALD sidewall treatments recovered the EQE of the 20×20 µm2 devices more than 150%. This indicated that AlGaInP µLEDs with ALD sidewall treatments can be used as the red emitter for full-color µLED display applications.