The Nd-Fe-B/Mo/Fe-Co multilayered films on MgO(001) were fabricated by UHV sputtering method. The as-deposited films showed soft magnetic properties with weak perpendicular magnetic anisotropy, and after annealing above 650°C, these films showed in-plane magnetic anisotropy, good squareness, and hard magnetic properties with high coercivity of about 8 kOe. The (220) peak of Nd2Fe14B was identified in the XRD pattern after annealing of the film, which means that the c-axis, which is the easy axis of magnetization, points in the plane of the film, consistent with the measurement of the magnetization curve. The positive peak of ΔM plot of in-plane direction of the film annealed at 800°C was shown. This result suggests existence of exchange coupling between the Nd-Fe-B and Fe-Co layers in the in-plane anisotropic multilayered film with monoatomic Mo interlayer.