In order to make GaN nanowires better used in the field of spin‐polarized electron sources, the structure and properties of transition metal (Cr, Mn, Fe, Co, and Ni) particles doped nanowires are studied through first principles. The research results show that transition metal (TM) particles are more likely to be doped on the outermost surface of GaN nanowires. The work function of Cr‐doped GaN nanowires has the largest decrease, which is 2.06 eV. For TM‐doped nanowires, magnetic moments are induced, which are mainly derived from the polarization of 3d electrons of TM atoms and 2p electrons of N atoms. Mn‐doped GaN nanowires with 100% spin polarization characteristics seem to be good candidates for spin‐polarized electron source photocathode applications.