Halloysite is a natural nanosized tubular clay mineral that has many potentially important uses in different industrial fields. In this paper, the key structural characteristics and properties of halloysite and their related applications are comprehensively reviewed. Research advances on halloysite, especially those from the past 20 years, are summarized with some critical comments. Attention is mainly paid to the structure and morphology of halloysite and their changes, the formation of tubular structures, the physicochemical properties, the surface chemical modifications, and the halloysite-based advanced materials and some related applications. Additionally, future prospects and key problems to be solved in halloysite studies are discussed. This review shed new light on both fundamental and applied studies that focused on halloysite.