Aloe vera (AV) gel has been widely used in various medical, cosmetic, and nutraceutical applications. However, AV rind, the tougher outer layer of AV leaves where the cell wall components exists, is currently treated as a fertilizer or waste. This study aimed to investigate the potential of the AV rind as a resource for the production of cellulose nanofibers. Since a detailed analysis of the AV rind has been lacking, chemical composition of rind was analyzed before processing it into nanofibers. The results showed that AV rind has a high proportion of α‐cellulose (57.72% ± 2.18%). AV rind nanofibers (AVRNF) were prepared using chemi‐mechanical process. The morphological analyses showed that most of the isolated fibers were individual fibers under 20 nm. Crystallinity and degree of polymerization of the obtained AVRNF, and mechanical properties of the nanofibrous film were evaluated and compared with the wood nanofibers. Tensile strength of AVRNF film (102 MPa) was comparatively lower than the wood fibers (132 MPa), which was consistent with the lower crystallinity of AVRNF [crystallinity index (CI) = 0.66] as well as the lower degree of polymerization (DP = 396), compared with wood fibers (CI = 0.90, DP = 1297). © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014, 131, 40592.