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Magnetic nanocomposites with 0-3 connectivity, whereby a 0D magnetic nanoparticle phase is embedded into a 3D magnetic metal matrix phase, have gained increased interest for use in applications ranging from integrated power inductor cores to exchange-spring magnets. The electro-infiltration process, in which a metal phase is electroplated through a nanoparticle film phase, is an inexpensive approach compatible with semiconductor fabrication methods for the formation of these nanocomposites. Past demonstrations of electro-infiltrated nanocomposites have relied on scanning electron microscopy and energy dispersive x-ray spectroscopy to evaluate the 0-3 composite structure. However, a detailed investigation of the boundary between the particle and metal matrix phases cannot be performed with these tools, and it is unknown whether the particle/matrix interfaces are dense and void-free. This detail is critical, as the presence of even nanoscale voids would affect any potential magnetic exchange coupling and hence the overall electromagnetic properties of the material. This work seeks to explore the phase boundary of 0-3 magnetic nanocomposite fabricated by electro-infiltration by using scanning transmission electron microscopy and energy-dispersive x-ray spectroscopy to analyze the nanostructure of two different composites—a nickel/iron-oxide composite and a permalloy/iron-oxide composite. High-resolution imaging indicates that the interface between the particle phase and matrix phase is dense and void-free. These results will help guide future studies on the design and implementation of these magnetic nanocomposites for end applications.