Optoelectronic effects of sidewall passivation on micro-sized light-emitting diodes (µLEDs) using atomic-layer deposition (ALD) were investigated. Moreover, significant enhancements of the optical and electrical effects by using ALD were compared with conventional sidewall passivation method, namely plasma-enhanced chemical vapor deposition (PECVD). ALD yielded uniform light emission and the lowest amount of leakage current for all µLED sizes. The importance of sidewall passivation was also demonstrated by comparing leakage current and external quantum efficiency (EQE). The peak EQEs of 20 × 20 µm µLEDs with ALD sidewall passivation and without sidewall passivation were 33% and 24%, respectively. The results from ALD sidewall passivation revealed that the size-dependent influences on peak EQE can be minimized by proper sidewall treatment.