Inosine pranobex (InP), an immunomodulatory drug approved for clinical use worldwide, is a potential adjuvant for cancer vaccines with a low clinical translation barrier. However, the administration of soluble InP agents in free format is associated with drawbacks of a short half-life period and limited efficacy. In this study, a rapid self-assembly approach was proposed for the synthesis of cancer vaccines due to the coordination interaction of ferric ion and acedoben (Ace) in InP. The self-assembled cancer vaccines can be readily adjusted from the microscale to the nanoscale, with shapes including rods, fibers, and spheres. Herein, Fe-Ace coordination complexes not only serve as carriers for tumor antigens, but also enhance antigen-specific antitumor immunity due to their intrinsic adjuvant properties. Nanofibrous self-assembled cancer vaccines based on Fe-Ace coordination complexes more effectively induced an antitumor immune response, exerted a remarkable therapeutic effect, and inhibited the tumor growth at distant site in vivo, compared to free InP and other self-assembled cancer vaccines. The presented work provides a promising strategy for the rapid manufacture of InP-derived self-adjuvant, self-carrier, and self-assembled vaccines for cancer immunotherapy.