Abstract: Thermoelectric properties of bulk and bilayer two-dimensional (2D) MoS₂/MoSe₂ heterostructures are investigated using density functional theory in conjunction with semiclassical Boltzmann transport theory. It is predicted that the bulk 2D heterostructures could considerably enhance the thermoelectric properties as compared with the bulk MoSe₂. The enhancement originates from the reduction in the band gap and the presence of interlayer van der Waals interactions. We therefore propose the 2D MoS₂/MoSe₂ heterostructures as a possible candidate material for thermoelectric applications.