We performed neutron-diffraction measurements on single crystals of La2-2xSr1+2xMn2O7. For x = 0.45, in an intermediate phase (TC < T < T-N), an antiferromagnetic (AFM) correlation gives rise to a diffuse signal along c with a period of 1/z(o) (z(o) similar to 0.2; the distance of Mn ions within a bilayer along c). Below T-C, however, the period of the diffuse signal changes due to the appearance of a canted AFM structure. These results indicate that a phase separation does not occur between a ferromagnetic (FM) and an AFM spin correlation along c.