Abstract: Acid mine drainage presents an important threat to cementitious structures. This study is aimed at investigating the effect of cellulose nanocrystals (CNCs) on the acid resistance of cementitious composites. CNCs were added to mortar mixtures as additives at cement volume ratios of 0.2vol%, 0.4vol%, 1.0vol%, and 1.5vol%. After 28 d of standard curing, the samples were immersed in a sulfuric acid with a pH value of 2 for 75 d. The unconfined compressive strength (UCS) test, the density, water absorption, void volume test, and thermogravimetric analysis were carried out to investigate the properties of CNC mixtures before sulfuric acid immersion. It was found that the addition of CNC reduced the volume of permeable voids and increased the hydration degree and mechanical strength of the samples. Changes in mass and length were monitored during immersion to evaluate the acid resistance of mixtures. The mixture with 0.4vol% CNC showed a reduced mass change and length change indicating its improved acid resistance.