Metal organic frameworks (MOFs) have been extensively applied in fields such as gas separation, catalysis, and energy, owing to their unique porous structure. However, the poor conductivity and chemical instability have limited their application in electrochemical energy such as lithium-ion batteries. Herein, we report self-supported nanorod arrays of multicomponent CPO-27 MOF grown on Ni foams as an efficient binder-free anode for lithium storage. The unique three-dimensional architecture design and multiple components endow the CPO-27 nanoarray with improved electron and ion transport, thus enabling a remarkable lithium storage performance. The CPO-27 array exhibits a high reversible capacity of 834 mA h g−1 at a rate of 50 mA g−1, and retains a capacity of 456 mA h g−1 at 1000 mA g−1 after 500 cycles. The architecture also shows a remarkable rate capability, affording a capacity of 440 mA h g−1 at a rate of 2000 mA g−1. This work offers innovative insights to design high-performance electrode materials of MOF compounds.