Bulk samples of La2−2xCa1+2xMn2O7with the layered Sr3Ti2O7‐type perovskite structure have been successfully synthesized and investigated with respect to their magnetic and electrical properties. It is found that La2−2xCa1+2xMn2O7(x=0.25) is a metallic ferromagnet with a magnetic transition temperatureTcof 215 K. The large magnetoresistance (MR) effect with &Dgr;&rgr;/&rgr;0of ∼60% at 1.8 T was observed in a wide temperature range below a cusp temperature in resistivity of 96 K, which is well below the magneticTc. This behavior is quite different from that of the well‐known double‐exchange ferromagnets such as La1−xCaxMnO3, where large MR effects are restricted to a narrow temperature range around the ferromagnetic transition. The present result could be interpreted by using the double‐exchange theory incorporating the anisotropy resulting from the two‐dimensional Mn‐O‐Mn networks in La2−2xCa1+2xMn2O7. ©1996 American Institute of Physics.