Cellulose biocomposites are widely used in industry as a low-cost engineering material with plant fiber reinforcement. However, chemical and microstructural heterogeneity causes low strength, low strain-to-failure, high moisture sensitivity, and odor and discoloration problems. Efforts toward improved performance through fiber orientation control, increased fiber lengths, and biopolymer use are reviewed. Interfacial strength control and moisture sensitivity are remaining challenges. As an attractive alternative reinforcement, high-quality cellulose nanofibers obtained by wood pulp fiber disintegration can be prepared at low cost. These nanofibers have high length/diameter ratios, diameters in the 5–15 nm range, and intrinsically superior physical properties. Wood cellulose nanofibers are interesting as an alternative reinforcement to more expensive nanoparticles, such as carbon nanotubes. Nanopaper and polymer matrix nanocomposites based on cellulose nanofiber networks show high strength, high work-of-fracture, low moisture adsorption, low thermal expansion, high thermal stability, high thermal conductivity, exceptional barrier properties, and high optical transparency. The favorable mechanical performance of bioinspired foams and low-density aerogels is reviewed. Future applications of cellulose biocomposites will be extended from the high-volume/low-cost end toward high-tech applications, where cellulose properties are fully exploited in nanostructured materials.