Selective catalysis remains a significant challenge owing to the lack of a generic protocol suitable for the preparation of selective catalytic materials. A promising approach is to translate the principle of enzyme catalysis for the design of new catalytic materials. Known as a “key-to-lock” technology, molecular imprinting provides a promising perspective by helping create in a straightforward manner binding sites that possess enzyme-like catalytic ability with but higher stability. In this chapter, we focus on discussing some key issues involved in active molecularly imprinted polymers from catalytic applications. The similarity and difference between preparing conventional molecularly imprinted polymers and catalytic imprinted polymers are highlighted. Other aspects relating to the principle, design, and future outlook of catalytic molecularly imprinted polymers are also discussed.