Due to the rapidly developing technologies and huge market demand, there has been increasing interest internationally in exploring permanent magnet formulations in addition to the well-known Nd2Fe14B and SmCo5/Sm2Co17. Given Fe's low materials cost and generally high magnetization, Fe-rich rare earth binaries such as Ce2Fe17 comprise a rich "hunting ground" for such new materials. While this compound suffers from a low ordering point and is a helimagnet, these difficulties are easily remedied by the substitution of appropriate amounts of cobalt for Fe, with room-temperature saturation magnetization as high as 1.5T. Here, we try to switch the all-important magnetic anisotropy from planar to uniaxial behavior in Ce2Fe17 via 18h- and 6c-type atom substitutions with Si, Ir, and numerous other atoms. The uniaxial magnetocrystalline anisotropy is successfully achieved in the 6c-site-substituted Ce2Fe15Ir2 systems, along with large magnetization. We find that iridium substitution, in particular, induces a substantial uniaxial anisotropy of 11.25 MJ/m(3), which is comparable to most of the current rare earth permanent magnets. Although the iridium substitution is costly, the finding of Ir-triggered uniaxial magnetic anisotropy indicates the potential of Ce-Fe-based alloys for permanent magnets.