We demonstrate a simple, facile approach to the deposition of silver nanoparticles on the surface of cellulose microfibrils with a quasi-one-dimensional arrangement. The process involves the generation of aldehyde groups by oxidizing the surface of cellulose microfibrils and then the assembly of silver nanoparticles on the surface by means of the silver mirror reaction. The linear nature of the microfibrils and the relatively uniform surface chemical modification result in a uniform linear distribution of silver particles along the microfibrils. The effects of various reaction parameters, such as the reaction time for the reduction process and employed starting materials, have been investigated by transmission electron microscopy (TEM) and ultraviolet−visible spectroscopy. Additionally, the products were examined for their electric current−voltage characteristics, the results showing that these materials had an electric conductivity of approximately 5 S/cm, being different from either the oxidated cellulose or bulk silver materials by many orders of magnitude.