Core‐shell structured nanocarriers have come into the scientific spotlight in recent years due to their intriguing properties and wide applications in materials chemistry, biology, and biomedicine. Tailored core‐shell structures to achieve desired performances has emerged as a research frontier in the development of smart drug delivery system. However, a systematic review on the design and loading/release mechanisms of stimulus‐responsive core‐shell structured nanocarriers is seldom available. This review starts with the categories of core‐shell structured nanocarriers with different means of drug payload, and then highlights the controlled release mechanism realized through stimulus‐response processes triggered under different environments. Finally, some multifaceted perspectives on the design of core‐shell structured materials as drug carriers are addressed. We hope this review could provide new enlightenments and prospects in the drug delivery field for further developing advanced and smart nanocarriers.This article is protected by copyright. All rights reserved