We have observed magnetic diffuse signals of the bilayer manganite La1.1Sr1.9Mn2O7 by neutron scattering. Even at the low temperature, 20 K, there is a diffuse signal, which is much stronger than that observed in the high temperatures, 144 and 288 K. This signal cannot be characterized by a bilayer structure as observed at 144 K nor by a monolayer structure as at 288 K, but by a high degeneracy of a canted spin structure. Thus, an observation of this diffuse signal is the direct evidence for the establishment of the canted spin structure in La1.1Sr1.9Mn2O7.