Background: A recent study suggested to develop and implement more interacted material for preprocedural education to decrease patients' anxiety about the atrial fibrillation (AF) ablation. This study compared the effectiveness of using either newly developed virtual reality (VR) materials (VR group) or paper-based materials (paper group) on giving AF preprocedural education. Methods: This study consequentially enrolled 33 AF patients preparing for ablation from November 2019 to October 2020. After enrollment, patients were randomized as either paper (n = 22) or VR (n = 11) groups. Results: In comparison with the baseline stage, at the posteducation stage, the degree of improvement in patients' self-assessed self-efficacy on AF ablation knowledge was higher among VR group patients than those in the paper group. At the posteducation stage, the patients' satisfaction to preprocedural education and used materials were higher among the VR group than that among the paper group. In addition to meet their needs and give accurate medical information, VR group patients reported that VR materials increased the effectiveness of education, increased their preparedness for AF catheter ablation, achieved paperless purposes, and willing to recommend VR materials to others. Operators subjectively reported that the periprocedure cooperation was increased both among paper and VR group patients after preprocedural education for the details of procedure. Better preparedness of VR group patients was supported by less periprocedure pain, anxiety, and impatience than those among paper group patients. Conclusion: Interactive VR-based materials are superior to the paper-based materials to provide patients immerse and imagine the journey and detail knowledge of AF catheter ablation before the procedure and better prepared patients for the procedure.