High-energy ball milling using comilling in a solid state by low-temperature mechanical alloying to prepare nickel-ferrite (NiFe2O4) nanopowders and ultrafine poly(methyl methacrylate) (PMMA), dispersing nanoparticles in a polymer matrix, and a uniaxial high-velocity cold compaction process using a cylindrical, hardened steel die and a new technique with relaxation assists have been studied. The focus has been on the particle size distributions of the nanocomposite powder during the milling and on the surface morphology of the nanocomposite-compacted materials after compaction with and without relaxation assists. Experimental results for different milling systems are presented showing the effects of milling time and material ratio. It was found that a longer mixing time give a higher degree of dispersion of the nanopowder on the PMMA particle surfaces. Furthermore, with increasing content of NiFe2O4 nanopowder, the reduction of the particle size was more effective. Different postcompacting profiles, i.e. different energy distributions between the upper and lower parts of the compacted powder bed, lead to different movements of the various particles and particle layers. Uniformity, homogeneity, and densification on the surfaces in the compacted powder are influenced by the postcompacting magnitude and direction. It was found that the relaxation assist device leads to an improvement in the polymer powder compaction process by reducing the expansion of the compacted volume and by reducing the different opposite velocities, giving the compacted composite bed a more homogeneous opposite velocity during the decompacting stage and reducing the delay time between the successive pressure waves.