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The combination of cellulose-based materials and functional polymers is a promising approach for the preparation of porous, biotemplated ceramic materials. Within this study, cellulose substrates were functionalized with a surface-attached initiator followed by polymerization of (3-methacryloxypropyl)heptaisobutyl-T8-silsesquioxane (MAPOSS) by means of surface-initiated atom transfer radical polymerization (ATRP). Successful functionalization was proven by infrared (IR) spectroscopy as well as by contact angle (CA) measurements. Thermal analysis of the polymer-modified cellulose substrates in different atmospheres (nitrogen and air) up to 600 ◦C led to porous carbon materials featuring the pristine fibre-like structure of the cellulose material as shown by scanning electron microscopy (SEM). Interestingly, spherical, silicon-containing domains were present at the surface of the cellulose-templated carbon fibres after further ceramisation at 1600 ◦C, as investigated by energy dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD) measurements.