A 100-nm-thick L21-ordered full-Heusler Co2FeSi (CFS) alloy film was fabricated using the facing targets sputtering (FTS) method at a substrate temperature TS of 300 ºC. The degrees of L21- and B2-order for the film were 37% and 96%, respectively. In addition, full-Heusler CFS alloy thin films with perpendicular magnetic anisotropy (PMA) induced by the magnetic anisotropy of MgO-interfaces were also successfully fabricated using the FTS method. The CFS/MgO stacked layers exhibited PMA when the CFS layer had a thickness of 0.6 nm ≤ dCFS ≤ 1.0 nm. The PMA in these structures resulted from the CFS/MgO interfacial perpendicular magnetic anisotropy.