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Metal vanadium phosphates (MVP), particularly Li₃V₂(PO₄)₃ (LVP) and Na₃V₂(PO₄)₃ (NVP), are regarded as the next-generation cathode materials in lithium/sodium ion batteries. These materials possess desirable properties such as high stability, theoretical capacity, and operating voltages. Yet, low electrical/ionic conductivities of LVP and NVP have limited their applications in demanding devices such as electric vehicles. In this work, a novel synthesis route for the preparation of LVP/NVP micro/mesoporous 3D foams via assembly of elastin-like polypeptides is demonstrated. The as-synthesized MVP 3D foams consist of microporous networks of mesoporous nanofibers, where the surfaces of individual fibers are covered with MVP nanocrystallites. TEM images further reveal that LVP/NVP nanoparticles are about 100–200 nm in diameter, with each particle enveloped by a 5 nm thick carbon shell. The MVP 3D …