Relationship between crystallographic orientation and ferromagnetic properties, especially, the squareness (the ratio of remanent magnetization against saturated magnetization, Mr/Ms) of epitaxial nickel zinc ferrite (Ni,Zn)Fe 2 O 4 (NZF) thin films were investigated. The orientation of NZF thin film was controlled by the amount of Al 2 O 3 content in (MgO-Al 2 O 3 )/CeO 2 /YSZ buffer layer on Si(001) substrate. ( 111)-oriented epitaxial NZF thin film had much higher Mr/Ms value than (001)-oriented one. It was clarified that maximum Mr/Ms value (around 82%) was obtained when the amount of Al 2 O 3 was 20-40 mol%. Atomic force microscope (AFM) and magnetic force microscope (MFM) observation revealed that high surface roughness and intense magnetic flux was observed when the amount of Al 2 O 3 was 20-40 mol%. The addition of SiO 2 into NZF was also tried, however, Mr/Ms value was not improved by the SiO 2 addition.