How do trees support their upright massive bodies? The support comes from the incredibly strong and stiff, and highly crystalline nanoscale fibrils of extended cellulose chains, called cellulose nanofibers. Cellulose nanofibers and their crystalline parts—cellulose nanocrystals, collectively nanocelluloses, are therefore the recent hot materials to incorporate in man‐made sustainable, environmentally sound, and mechanically strong materials. Nanocelluloses are generally obtained through a top‐down process, during or after which the original surface chemistry and interface interactions can be dramatically changed. Therefore, surface and interface engineering are extremely important when nanocellulosic materials with a bottom‐up process are fabricated. Herein, the main focus is on promising chemical modification and nonmodification approaches, aiming to prospect this hot topic from novel aspects, including nanocellulose‐, chemistry‐, and process‐oriented surface and interface engineering for advanced nanocellulosic materials. The reinforcement of nanocelluloses in some functional materials, such as structural materials, films, filaments, aerogels, and foams, is discussed, relating to tailored surface and/or interface engineering. Although some of the nanocellulosic products have already reached the industrial arena, it is hoped that more and more nanocellulose‐based products will become available in everyday life in the next few years.

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Cellulose nanofibrils (CNFs) and single-walled carbon nanotubes (SWNTs) hold potential for fabricating multifunctional composites with remarkable performance. However, it is technically tough to fabricate materials by CNFs and SWNTs with their intact properties, mainly because of the weakly synergistic interaction. Hence, constructing sturdy interfaces and sequential connectivity not only can enhance mechanical strength but also are capable of improving the electrical conductivity. In that way, we report CNF/SWNT filaments composed of axially oriented building blocks with robust CNF networks wrapping to SWNTs. The composite filaments obtained through the combination of three-mill-roll and wet-spinning strategy display high strength up to ∼472.17 MPa and a strain of ∼11.77%, exceeding most results of CNF/SWNT composites investigated in the previous literature. Meanwhile, the filaments possess an electrical conductivity of ∼86.43 S/cm, which is also positively dependent on temperature changes. The multifunctional filaments are further manufactured as a strain sensor to measure mass variation and survey muscular movements, leading to becoming optimistic incentives in the fields of portable gauge measuring and wearable bioelectronic therapeutics.