A key challenge in realizing ultrahigh-resolution displays is the efficient preparation of ultrasmall-sized (USS) light-emitting diodes (LEDs). Today, GaN-based LEDs are mainly prepared through dry etching processes. However, it is difficult to achieve efficient and controllable etching of USS LED with high aspect ratios, and LED sidewalls will appear after etching, which will have a negative impact on the device itself. Herein, a method for preparing USS LED based on GaN epitaxial wafers is reported (on two types of wafers, i.e., with p-GaN fully activated and unactivated). F-ions are injected into the intentionally exposed areas on the two types of wafers to achieve device isolation. The area under the micro-/nano-sized protective masks (0.5, 0.8, 1, 3, 5, 7, 9, and 10 µm wide Ni/Au stripes) are the LED lighting areas. The LED on the p-GaN unactivated wafer (UAW) requires further activation. The Ni/Au mask not only serves as the p-electrode of LED but also Ni as a hydrogen (H) removing metal covering the surface of p-GaN UAW that can desorb H from a Mg element in the film at relatively low temperatures, thereby achieving the selective activation of LED lighting areas. Optoelectronic characterization shows that micro-/nano-sized LED arrays with individual-pixel control were successfully fabricated on the two types of wafers. It is expected that the demonstrated method will provide a new way toward realizing ultrahigh-resolution displays. Analyzing the changes in the current flowing through LED (before and after selective activation) on the F-injected p-GaN UAW, it is believed that depositing H removing metal on p-GaN UAW could possibly realize the device array through the selective activation only (i.e., without the need for ion implantation), offering a completely new insight.