Recently, development of a new type of anode material for lithium-ion batteries that possesses multielectron reaction, sufficient charge transfer, and restricted volume suppression has been considered a huge challenge. Herein, we find a simple hot-pressing method to incorporate polyoxometalate (POM)-based metal-organic frameworks (MOFs) onto three-dimensionally structured carbon cloth (CC), denoted as HP-NENU-5/CC, which immobilizes POMs into the MOFs avoiding the leaching of POMs and employs HP-NENU-5/CC as a flexible, conductive, and porous anode material. The HP-NENU-5/CC anode materials show outstanding electrochemical performance, exhibiting high reversible capacity (1723 mAh g(-1) at 200 mA g(-1)), high rate capability (1072 mAh g(-1) at 1000 mA g(-1)), and superior cycling stability (1072 mAh g(-1) at 1000 mA g(-1) after 400 cycles). Most importantly, the performance of HP-NENU-5/CC is the best among those of all reported POMs and MOF-based materials. In addition, we perform a comparative study for active materials coated on a two-dimensional current collector and CC, and our experimental results and analysis prove that the active material coated on CC does enhance the electrochemical performance.