The interlayer coupling and magnetization reversal behaviors in NiFe/NiO/NiFe trilayers were investigated using polarized neutron reflectivity and Monte Carlo (MC) simulations. Our results reveal that the shape of NiFe loops transitions from square to tilted as the NiO thicknesses decrease, indicating changes in the direction of NiFe layer’s easy axis. This phenomenon can be attributed to variations occurring at NiO/NiFe interfaces for different NiO layer thicknesses. With thin NiO layer, interdiffusion at the NiO/NiFe interfaces leads to frustrated coupling, resulting in a noncollinear interlayer coupling. This observation is supported by MC simulations. Conversely, hardly any coupling frustration is observed for the sample with a thick NiO layer. Our findings propose a novel way to tailor the interlayer coupling through interface engineering.