Large and variable in-plane uniaxial magnetic anisotropy in a nanocrystalline (Co2FeAl)97.8(Al2O3)2.2 soft magnetic thin film is obtained by an oblique sputtering method without being induced by magnetic field or post annealing. The in-plane uniaxial magnetic anisotropy varies from 50 Oe to 180 Oe (1 Oe = 79.5775 Am−1) by adjusting the sample's position. As a result, the ferromagnetic resonance frequency of the film increases from 1.9 GHz to 3.75 GHz.