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We study the perpendicular magnetic anisotropy in (Fe100−xNix)80B20 (FeNiB) films with various Ni contents. Perpendicularly magnetized films are achieved when the Ni content is in the range of 30 at. %–70 at. %. An effective perpendicular magnetic anisotropy (PMA) constant of 1.1× 105 J/m3 is achieved for the (Fe50Ni50)80B20 film. We also fabricate magnetic tunnel junction devices containing FeNiB films, and electrical measurements show that a tunneling magnetoresistance ratio of more than 20% can be achieved for devices having an orthogonal magnetization configuration. The PMA of the FeNiB film clearly changes by varying the bias voltage applied along the FeNiB/MgO junction, and a voltage-controlled magnetic anisotropy (VCMA) efficiency of over 30 fJ/Vm is demonstrated. From systematic investigations, there is no clear correlation between PMA and VCMA efficiency in the FeNiB/MgO junction. These experimental results should facilitate the development of energy-efficient magnetic random-access memory.