Creating artificial enzymes that mimic the complexity and function of natural systems has been a great challenge for the past two decades. In this Progress Report, the focus is on recently discovered “hidden talents” of gold nanomaterials in artificial enzymes, including mimicking of nuclease, esterase, silicatein, glucose oxidase, peroxidase, catalase, and superoxide dismutase. These unexpected enzyme-like activities can be ascribed to nano-gold itself or the functional groups present on surrounding monolayer. Along with introducing the mechanisms of the various enzyme-like activities, the design and development of gold-based biomimetic catalysts, the search for efficient modulators, and their potential applications in bionics, biosensing, and biomedical sciences are highlighted. Eventually, it is expected that the rapidly growing interest in gold-based nanozymes will certainly fuel the excitement and stimulate research in this highly active field.