In recent years, researchers are developing novel nanoparticles for diagnostic applications using imaging techniques and for therapeutic purposes through drug delivery techniques. The unique physical and chemical properties of mesoporous silica nanoparticles (MSNs) make it possible to integrate a variety of commonly used therapeutic and imaging agents to construct a multimodal synergistic anticancer drug delivery system. Here, we review recent advances in MSNs synthesis for drug delivery and smart response applications. First, we outline synthetic strategies for the fabrication of ordered MSNs, hollow MNSs, core-shell structured MSNs, dendritic MSNs, and biodegradable MSNs. Then, the recent research progress in designing functional MSN materials with various controlled release mechanisms in anticancer therapy is discussed, and new properties are introduced to suggest the latest design requirements as drug delivery materials. The review also highlights significant achievements in bioimaging using mesoporous silica nanoparticles and their multifunctional counterparts as delivery vehicles. Finally, we present our personal views on key directions for future work in this area. This article is protected by copyright. All rights reserved.