On the basis of nanocellulose obtained by acidic swelling and ultrasonication, rodlike nanocellulose/polyaniline nanocomposites with a core-shell structure have been prepared via in situ polymerization. Compared to pure polyaniline, the nanocomposites show superior film-forming properties, and the prepared nanocomposite films demonstrate excellent electrochemical and electrochromic properties in electrolyte solution. Nanocomposite films, especially the one prepared with 40% polyaniline coated nanocomposite, exhibited faster response time (1.5 s for bleaching and 1.0 s for coloring), higher optical contrast (62.9%), higher coloration efficiency (206.2 cm/C), and more remarkable switching stability (over 500 cycles). These novel nanocellulose-based nanorod network films are promising novel electrochromic materials with excellent properties.