Copper zirconium phosphate nanoparticles have been used as an efficient catalyst for the acetyla‐tion of a wide range of alcohols and phenols with acetic anhydride in good to excellent yields under solvent‐free conditions. The steric and electronic properties of the different substrates had a signif‐icant influence on the reaction conditions required to achieve the acetylation. The catalyst used in the current study was characterized by inductively‐coupled plasma optical emission spectroscopy, energy dispersive spectroscopy, X‐ray diffraction, N2 adsorption‐desorption, scanning electron microscopy, and transmission electron microscopy. These analyses revealed that the interlayer distance in the catalyst increased from 7.5 to 8.0 ? when Cu2+was intercalated between the layers, whereas the crystallinity of the material was reduced. This nanocatalyst could also be recovered and reused at least six times without any discernible decrease in its catalytic activity. This new method for the acetylation of alcohols and phenols has several key advantages, including mild and environmentally friendly reaction conditions, as well as good to excellent yields and a facile work‐up.