In uniaxially stretched films, the refractive indices perpendicular to the stretching direction have the same value, and so, the out-of-plane birefringence is half that of the in-plane birefringence. This means that these values cannot be controlled independently in uniaxially stretched films. The same relationship was previously observed when needle-shaped nanoparticles were added to uniaxially stretched films. This paper presents a method to achieve the three-dimensional birefringence control of uniaxially stretched films. When we added plate-shaped smectite nanoparticles to uniaxially stretched films, different relationships were observed for the in- and out-of-plane birefringence. The magnitude of the out-of-plane birefringence increased more than would be expected according to the usual relationship. According to our results, uniaxially stretched films with no out-of-plane birefringence and negative in-plane birefringence can be formed by adding smectite nanoparticles to polymer films with negative in-plane birefringence. Using our method, the three-dimensional birefringence of uniaxial polymers can be controlled, and the possibility of the uniaxial films could be drastically extended.