This study is devoted to the luminescence and stimulated emission properties of the ZnO hybrid structure, which is vertically aligned microcrystals with the [0001] crystallographic orientation and a pronounced hexagonal shape formed on a continuous layer of micron thickness. These microcrystals are up to 10 µm high and up to 8 µm in diameter and form the main part of the structure’s thickness. The structure was synthesized on the M(101¯0) plane of sapphire using the magnetron sputtering method. Luminescence of the structure, represented only by conventional near-UV and green components under low-intensity continuous photoexcitation, confirms its high structural and optical quality. Under pulsed photoexcitation with relatively high intensity, stimulated emission (SE) was observed from the structure in the near-UV region at room temperature. The threshold power density for SE was 0.1–0.2 MW/cm2. Exceeding the threshold leads to a significant increase in the emission intensity compared to the control film without [0001] microcrystals, also grown on M(101¯0) sapphire. It was assumed that the optical gain is provided by the whispering gallery modes of individual [0001] microcrystals as a result of inelastic exciton–electron scattering, at least at near-threshold excitation intensities.