Chromium selenide thin films were grown epitaxially on Al2O3(0001) and Si(111)-(7×7) substrates using molecular beam epitaxy (MBE). Sharp streaks in reflection high-energy electron diffraction and triangular structures in scanning tunneling microscopy indicate a flat smooth film growth along the c-axis, and is very similar to that from a hexagonal surface. X-ray diffraction pattern confirms the growth along the c-axis with c-axis lattice constant of 17.39 Å. The grown film is semiconducting, having a small band gap of about 0.034 eV, as calculated from the temperature dependent resistivity. Antiferromagnetic nature of the film with a Néel temperature of about 40 K is estimated from the magnetic exchange bias measurements. A larger out-of-plane exchange bias, along with a smaller in-plane exchange bias is observed below 40 K. Exchange bias training effects are analyzed based on different models and are observed to be following a modified power-law decay behavior. as observed from neutron diffraction studies [6][7][8][9]. Because of Cr vacancies in alternate layers, the moment associated with Cr atoms located on two different layers are different due to different neighboring environment and this leads to the complexity in the magnetic structure below TN.Previously, chromium selenide systems have been studied to investigate their suitability as thermoelectric material for intermediate-temperature applications [10][11][12][13][14], intermediate temperature power generation [13], electrochemical sensors [15], etc. Several groups have studied the structural, magnetic, electrical and thermoelectric properties of single crystal Cr2+xSe3-x compounds grown using solid state reaction method [10][11][12][13]16], soft chemical and hydrothermal synthesis [15,17,18] and chemical vapor transport method [4,14,[19][20][21]. However, the studies focus mostly on the improvement in thermoelectric properties of transition-metal-doped bulk samples of Cr2Se3. The epitaxial growth and different physical properties of Cr2Se3 thin films are yet to be explored in detail. Molecular beam epitaxy (MBE) is a highly specialized technique used to grow ultra-high purity large-area epitaxial thin films with abrupt interfaces and with precise control over their thicknesses. Compared to other growth techniques, MBE offers greater control to incorporate dopants in thin films. This makes it even more suitable growth method, as the electrical, magnetic and thermoelectric properties of this material system can be largely varied with addition of transition-metal/chalcogen dopants [1, 9-13, 21,22].In this work, we report the epitaxial growth of Cr2Se3 thin films under ultra-high vacuum (UHV) directly on Al2O3(0001) and Si(111)-(7×7) surfaces using MBE. Interestingly, we show that the growth occurs along (001) direction (c-axis). We present the details of growth, structural, electrical and magnetic properties characterized by several in situ and ex situ techniques, e.g., reflection high energy electron diffraction (RHEED), x-ray diffraction (XRD), scanning...