The invention discloses a novel technology for Bayer process-based separation of iron in high-iron red mud. The novel technology comprises the following steps of A, carrying out sedimentation on alumina production solid waste, washing bottom-flow red mud three times, carrying out roughing separation by a vibrating screen, adding water into the red mud so that red mud solid content satisfies magnetic separation requirements, and at least carrying out a magnetic separation process to separate concentrate and mine tailing, B, carrying out concentration on the concentrate, carrying out overflow separation to remove most water, and carrying out press filtration to obtain filter cake which is iron concentrate, and C, carrying out concentration on the mine tailing, carrying out overflow separation to remove most water, carrying out press filtration to obtain filter cake and carrying out dry-type stockpiling. The invention discloses a device for Bayer process-based separation of iron in high-iron red mud. The device comprises a buffer slot, the vibrating screen, a magnet separator, a concentrate tank, a mine tailing tank, a concentration machine and a filter press. The device matches the novel technology, has a high yield and a high total iron recovery rate and utilizes a mine tailing dry-type stockpiling process. The novel technology has a simple process, is mature in operation and realizes production easily.