The degree of coverage and the structure and thickness of interphases in composite latex particles consisting of a poly(butyl acrylate) (PBA) core incorporated with poly(methyl methacrylate) (PMMA) macromonomer of different molecular weight and a PMMA shell was analyzed by using solid‐state NMR spin‐diffusion measurements. By changing the temperature at a given filter strength or by adjusting the filter strength at a given temperature, the spin‐diffusion experiment could be performed in such a way that the overall structure could be detected. At filter strengths softer than necessary for the detection of the overall structure, information regarding larger structures can be obtained, whereas for stronger filters detailed information about small structures in the interphase region can be extracted. The data obtained by NMR were related to previous TEM and dynamic mechanical studies on these particles.