Here, we develop a robust approach to forming an ∼8 nm thick cellulose nanofiber (CNF) shell on polymer microparticles through an emulsion-templated assembly. The median diameter of the CNF-shelled microparticles was 3.0 μm. The microparticles showed good dispersibility in water with a ζ-potential of -46.7 ± 0.5 mV and had good mechanical resistance. The surface CNF shells showed pH-sensitive drug loading/releasing properties, which suggest potential for a range of therapeutic and biomedical applications.