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Flexible, pressure-sensitive composites can be prepared through the inclusion of electrically conductive particles as functional fillers into an elastomeric polymer matrix, which have been used for the applications of wearable devices for health monitoring and electronic skins. A key challenge associated with these composites is developing anisotropic pressure sensitivity while retaining their flexibility (or low filler content). Herein, we demonstrate a simple and scalable method for aligning anisotropic nickel-coated carbon fibers (NiCF) along with the thickness direction of a polymer matrix by applying a magnetic field. The aligning mechanisms and kinetics of NiCF in the polydimethylsiloxane (PDMS) precursor are revealed by in situ optical microscopy images while a magnetic field is applied. The aligned nickel-coated carbon fibers in the polymer effectively endow the composite films excellent pressure-sensitive performance. The pressure sensitivity of NiCF/PDMS composite films has been systematically studied and can be used for biological monitoring. We believe that this magnetic field assisted processing strategy provides a promising material solution for manufacturing fiber embedded polymer composites with enhanced pressure sensitivity, which is essential for future wearable health monitoring electronics and electronic skin.