Two distinct lignocellulosic fractions (rind and core) can be obtained through a physical separation of sugarcane stalks. Although presenting differences in morphology, both fractions can be employed to produce pulps and papers. The pulps and paper sheets produced from the core and rind fractions were characterized by their chemical composition, physical properties and mechanical properties. The pulps obtained from the core presented a higher amount of fines, lower drainage ability and rendered denser and stiffer sheets. The pulps from the rind, which have a higher content of fibers and higher degree of polymerization, produced sheets with higher air permeability and water absorption. Both paper sheets presented mechanical and physical properties comparable to commercial papers and papers from different cellulosic sources. The different properties exhibited by the papers produced from each fraction allow their use for distinct purposes, and expands the opportunities in the context of sugarcane biorefinery.