Abstract: The nanoparticle(NP)/polymershelled capsules possess both the sizedependent physiochemical properties of NPs and biomedical functions, such as encapsulation, protection and transportation of medical molecules, due to their unique composition and structures. Therefore, they are of great potential in many applications, especially in biomedical fields. Recent developed preparation methods and the properties of the templatefree selfassembled capsules are summarized and reviewed. The mechanisms of the capsules formation using the templatefree technique are illustrated. Compared to the well established layerbylayer (LBL) selfassembly approach, the templatefree selfassembly approach don′t need the removal of the templates during the synthesis of the NP/polymershelled hybrid capsules, which greatly simplify the approach. Various NPs were assembled into the capsules to endow the capsules unique properties, such as optical, magnetic, and catalytic properties, which hold great potential in biomedical fields.