In this dissertation, new ways for controlling the internal structures of a system of polymer composites, polymer blends, and hydrogel composites by means of external electric or magnetic fields are presented. The first part of this study addresses the development of an anisotropic phase-separated morphology in polymer blends by using electrically pre-oriented clay particles. It was observed that electrically pre-oriented montmorillonite clay particles in a homogenous single-phase blend lead to anisotropic phase-separated morphology of the blends, undergoing demixing upon temperature shift to a two-phase regime. The initial co-continuous microstructure developed into a coarsened and directionally organized phase-separated morphology parallel to the direction of oriented clay particles (applied AC electric field direction) over the annealing time. It was also found that the degree of clay orientation under AC electric field was linearly proportional to the degree of polymer-phase orientation. The temporal morphological evolution was thoroughly analyzed by electron microscopy and X-ray diffraction studies. The second part of the study covers anisotropic hydrogel nanocomposites developed by orienting magnetically sensitive nontronite clay minerals under the strong magnetic fields. Anisotropic hydrogel nanocomposites were formed by magnetic-field assisted orientation of nontronite clays suspended in a hydrogel precursor solution followed by a gelation process. The degree of orientation of nontronite minerals was quantitively characterized by birefringence and small-angle X-ray scattering. The resultant hydrogels exhibited anisotropic optical, mechanical, and swelling properties along the direction of oriented clay minerals. Anisotropic water swelling behaviors can be particularly applied in medical dressing materials, where vertical wicking of fluid into the wound dressing is sought after for minimizing periwound maceration damage.