In this article, we employ the multistate iterative Boltzmann inversion (MS-IBI) method to develop coarse-grained potentials capable of representing molecular structure in both the amorphous and crystalline phases of semicrystalline polymers with improved accuracy while allowing for tunable control over the dynamics governing the α-relaxation process. A unique feature of this method is that the potentials are blended using the product of the target structural distributions, for example, the radial density function, for each phase and a weighting factor. To demonstrate this approach, a family of potentials for polyethylene is developed where the weighting factor of the crystalline phase ranges is varied from zero, incorporating information only from the amorphous phase, to unity, where the model is trained from only the crystalline phase. The most accurate representation of structural distributions was obtained when the crystalline phases is weighted at 50%. However, we show that when the crystalline phase is weighted at 90%, the model more accurately represents dynamics of the α-relaxation process, with realistic predicted values of activation energy and diffusion rates, with relatively minor impact on accuracy in structure.