Chitin nanofiber (ChNF) has received significant research attention owing to its potential for use in a variety of applications, such as medicine and cosmetics. Here, we synthesize a novel ChNF material, ChNF-coated polymer microparticles, using a Pickering emulsion-templated approach. Two varieties of ChNF with different crystal structures, lengths, and surface charges were used to form the microparticle shells. When ChNFs with a shorter length and greater surface charge were used, the microparticles showed good dispersibility in water and narrow size distribution with number- and volume-median diameters of 1.46 and 1.84 μm, respectively. The microparticles were easily collected by filtration and redispersed in water, even after drying. The surface ChNF shells assembled at the microparticle surfaces showed potential as an adsorption site, effectively capturing anionic dye molecules. This technique offers new opportunities for the development of green nanocomposite materials using a facile aqueous process.