The effect of hydrogenating process on the homogeneity of hydrogen absorption in the La0.8Ce0.2(Fe1−xMnx)11.5Si1.5 compounds was investigated. It is attractive that the distribution of hydrogen atoms in the compounds becomes more uniform with increasing hydrogen pressure and annealing temperature. Homogeneous hydrides of La0.8Ce0.2(Fe0.985Mn0.015)11.5Si1.5 were obtained by annealing them at the temperature of 773 K and under the hydrogen atmosphere of 0.5 MPa. With changes of Mn content, the Curie temperatures (TC) of the hydrides of La0.8Ce0.2(Fe1−xMnx)11.5Si1.5 can be adjusted in the room temperature range from 279 to 312 K. Large magnetic entropy changes due to the itinerant-electron metamagnetic transition are obtained in the room temperature range for the hydrides of La0.8Ce0.2(Fe1−xMnx)11.5Si1.5.