Artificial nanoenzymes based on metal nanoclusters have received great attention for multienzyme activities nowadays. In this work, pepsin-capped copper NCs (Cu-Pep NCs) are used as oxidase, ascorbic acid oxidase (AAO), and peroxidase mimics, and their activities are enhanced by the introduction of imidazole. The oxidase activity increased almost 7.5-fold, while 5-fold and 2-fold increases were observed for the peroxidase and AAO-like activity, respectively. The enhanced radical formation in the presence of imidazole moieties facilitates the enzymatic activity of the Cu-Pep-NCs/Imid system. This work describes the different enzymatic activities of the NCs, paving a new way for artificial nanoenzymes having enhanced activities.