[en] Highlights: • Vertical heterostructure growth of n-MoS₂/p-MoS₂/p-GaN is demonstrated. • Vertical heterostructure of n-MoS₂/p-MoS₂/p-GaN is used to generate white light. • The n-MoS₂/p-MoS₂/p-GaN heterostructure can be used to fabricate energy saving LED. Despite the dramatic advances of two-dimensional vertical heterostructure, the controlled growth and potential applications in light emitting devices of these heterostructures have not yet been well established. Here, we report, for the first time, the epitaxial growth of two-dimensional p-MoS₂/n-MoS₂ vertical heterostructures by a chemical vapor deposition (CVD) method, where the n-MoS₂ was synthesized first, followed by an epitaxial growth of p-MoS₂ on top of the n-MoS₂ via a control of the growth temperature. Atomic-resolution scanning transmission electron microscopy (STEM) imaging reveals that the vertically stacked bilayer of the hexagram-shaped p-MoS₂/n-MoS₂ preferred the 2H stacking phase during the growth. The structural and optical features of the as-grown p-MoS₂/n-MoS₂ heterostructure were examined by Raman and photoluminescence (PL) spectroscopy. This novel hybrid heterostructure was demonstrated to be an excellent building block for a highly efficient white light emitting diode (WLED). In addition, we transferred the p-MoS₂/n-MoS₂ on top of a p-GaN bilayer to fabricate a tetra-layered (4-L) n-MoS₂/p-MoS₂/p-GaN heterostructure, which could emit electroluminescence (EL) in forward bias. The EL spectra comprise three emission peaks centered at 481 nm (from p-GaN), 525 nm (from p-MoS₂), and 642 nm (from n-MoS₂), with a dominant emission peak located at 642 nm. The WLED device composed of the n-MoS₂/p-MoS₂/p-GaN heterostructure showed a luminance of 30,548 cd/m², luminescence efficiency of 29% and the luminous efficacy of 294 lm/W at a bias voltage of 4 V. This work demonstrates that white light emission can be generated from vertically stacked few-layered 2D materials-based heterostructures, which also hold great potential for constructing color-tunable light emitters for low-cost display, lighting, and optical communication.