of TMDs alter with the layer thickness, ranging from single to few monolayers to bulk. The individual layers in the crystalline structure of atomically thin TMD (consisting of single or few layers) are held together by weak van der Waals force of attraction. [11,12] The absence of dangling bonds allows the fabrication of LMCs on various substrates or materials with different dimensionalities due to relaxation in strain related issues which arise due to lattice mismatch and thermal mismatch between the epitaxial layer and the substrate. [13] This opens the perspectives for the development of high-quality heterojunction devices based on LMCs and 3-dimensional semiconductors as the performance of such devices depend primarily on interfacial properties. Broadband photodetection can be achieved by integrating LMCs and other bulk semiconductors to cover the wide spectrum range.Various TMDs based on metals like Molybdenum (Mo), Tungsten (W), and Tin (Sn), such as MoS 2 , MoSe 2 , WS 2 , WSe 2 , SnS 2 , etc. have emerged as promising candidates for futuristic applications. [14][15][16][17][18][19][20][21] Among them, MoS 2 has been extensively studied in the past few years for TMD-based photodetectors due to its high sensitivity, light absorption, electron mobility, and lower dimensionality. [22][23][24] On a par with MoS 2 , MoSe 2 is another TMD that possesses great potential. MoSe 2 has a variable bandgap according to its number of layers, ranging from a direct bandgap of 1.6-1.9 eV for monolayer to an indirect bandgap of 1.1 eV for bulk. [25][26][27] It shows n-type conducting channel behavior with average mobility of 50 cm 2 V -1 s -1 for its monolayer-based field-effect transistors (FETs) whereas charge mobility of 100 cm 2 V -1 s -1 has been reported for bulk MoSe 2 . [28] More notably, its absorption spectrum spans the visible to nearinfrared (NIR) wavelength spectrum. However, the performance of MoSe 2 -based photodetectors is still circumscribed in terms of responsivity, detectivity and time response. [29][30][31][32][33] The proficiency of these photodetectors can be improvised by employing the heterostructure architecture. [28,[34][35][36] Furthermore, the combination of photoactive MoSe 2 and bulk semiconductor such as silicon (Si), germanium (Ge), Gallium nitride (GaN), or other compound semiconductors can provide high-performance broadband photodetectors by exploiting the advantageous properties of both the materials. Few research groups have demonstrated the MoSe 2 /Si [28,37,38] and MoSe 2 /Ge [36] heterojunction devices that showed responsivity ranging from 270 mA W −1 Heterojunction photodiodes comprising of layered metal chalcogenides and wide-bandgap semiconductors are a promising candidate for broadband photodetection. In this work, nanolayered Molybdenum diselenide (MoSe 2 )/Gallium Nitride (GaN) based photodetector has been demonstrated from ultraviolet to near-infrared range (300-1000 nm). The performance is investigated by conducting Kelvin probe force microscopy to measure the conduction band o...