A catalyst determines the mechanism of an organic chemical reaction, thus enabling the commercially viable formation of desired material products. Biopolymers offer new opportunities for the construction of catalysts by virtue of their biocompatibility, environmental benignity, and sustainability, as well as their low cost. Biopolymers are especially useful as carriers and precursors in catalysis application. The employment of biocompatible and biosustainable collagen and silk fibroin materials will revolutionize state-of-the-art electronic devices and systems that currently rely on conventional technologies. In this review, we first consider the ordered hierarchical structure, origin, and processing methods of collagen and silk fibroin. Then, the unique advantages and applicability of collagen and silk fibroin for constructing catalysts are summarized. Moreover, a summary of the state-of-the-art design, fabrication, and application of collagen- and silk fibroin-based catalysts, as well as the application of collagen- and silk-based catalysts, is presented by focusing on their roles as carriers and precursors, respectively. Finally, challenges and prospects are assessed for the construction and development of collagen and silk fibroin-based catalysts.