ZnCoO:H and ZnCoAlO:H films were synthesized by radio frequency magnetron sputtering in a (1 − x)Ar + xH2mixed atmosphere with x = 0.2–0.5. The films contain different amounts of metallic Co particles (from 7.6% and higher) ~4–7 nm in size. The magnetic and magneto-optical (MO) behavior of the films was analyzed in combination with their structural data. The samples exhibit high values of magnetization (up to 377 emu/cm3) and MO response at room temperature. Two situations are considered: (1) the film magnetism is associated only with isolated metal particles and (2) magnetism is present both in the oxide matrix and in metal inclusions. It has been established that the formation mechanism of the magnetic structure of ZnO:Co2+is due to the spin-polarized conduction electrons of metal particles and zinc vacancies. It was also found that in the presence of two magnetic components in the films, these components are exchange-coupled. In this case, the exchange coupling generates a high spin polarization of the films. The spin-dependent transport properties of the samples have been studied. A high value of the negative magnetoresistance of the films at room temperature (~4%) was found. This behavior was explained in terms of the giant magnetoresistance model. Thus, the ZnCoO:H and ZnCoAlO:H films with high spin polarization can be considered as sources of spin injection.