Optical manipulation of the magnetic anisotropy is demonstrated for bilayered manganites, La2-2xSr1+2xMn2O7, by means of femtosecond Kerr-rotation measurements. Upon the photoexcitation on the x=0.32 crystal, the magnetization exhibits the precessional motion for about 1 ns, revealing the directional change of the magnetocrystalline anisotropy from the c axis to the ab plane. This change of the anisotropy induces the nonthermal decrease of the c-axis magnetization component for about 1 ns.