High-anisotropy NiAs-type MnBi films are produced by in situ annealing of Bi/Mn/Bi trilayers, [Bi/Mn/Bi] n multilayers, and subsequent magnetic field annealing. Phase components, crystallographic anisotropy, and magnetic properties of the Mn x Bi 100Àx thin films exhibits strong dependence on Mn concentration. High-purity MnBi thin films with perfect c-axis orientation are obtained by carefully controlling the Mn/Bi ratio. An energy product of 16.3 MGOe, which is the highest value reported so far, is achieved for the x ¼ 50 film of thickness t ¼ 100 nm. The MnBi thick film (t ¼ 2 mm) changes from isotropic to anisotropic after magnetic field annealing. Depending on the direction of the applied field during magnetic field annealing, the MnBi thick film may have out-of-plane or in-plane anisotropy. This control of anisotropy direction enables applications of MnBi films in permanent-magnet, spintronic devices, or magnetic micro-electro-mechanical systems. In addition, the room-temperature magnetocrystalline anisotropy constant and saturation polarization of the hard magnetic MnBi phase are determined to be K ¼ K 1 þ K 2 ¼ 15.0 Mergs cm À3 and J s ¼ 8.2 kG, respectively.