Abstract Congenital heart defects (CHDs) are one of the most common congenital malformations, accounting for ≈30% of all congenital malformations. Interventional implantation of occlusion devices is becoming the preferred treatment for CHDs. However, current occlusion devices suffer from serious problems, such as thrombosis, slow endothelialization, imprecise localization, abrasion, displacement, etc. Here, a multifunctional drug‐carrying fiber platform with structural similar to the extracellular matrix is innovatively designed to develop 4D printed cardiac occlusion devices, with characteristics of efficient anticoagulation, proendothelialization, and precise localization. Biomimetic ligament structures are designed to achieve a similar mechanical response to myocardial tissue, which helps to synergize deformation and reduce tissue wear. A structural design method for biomimetic personalized multilevel occlusion devices is proposed, facilitating further improvement of sealing reliability. The radiopaque 4D printed shape memory composites are developed, realizing the complete visualization and precise localization of the device in vivo. The novel 4D printed cardiac occlusion device provides an effective way to reduce the risk of complications and contributes to versatility. It is expected to be a next‐generation multifunctional repair device for personalized treatment of CHDs.