We propose a facile method for synthesizing a novel Si membrane structure with good mechanical strength and three-dimensional (3D) configuration that is capable of accommodating the large volume changes associated with lithiation in lithium ion battery applications. The membrane electrodes demonstrated a reversible charge capacity as high as 2414 mAh/g after 100 cycles at current density of 0.1 C, maintaining 82.3% of the initial charge capacity. Moreover, the membrane electrodes showed superiority in function at high current density, indicating a charge capacity >1220 mAh/g even at 8 C. The high performance of the Si membrane anode is assigned to their characteristic 3D features, which is further supported by mechanical simulation that revealed the evolution of strain distribution in the membrane during lithiation reaction. This study could provide a model system for rational and precise design of the structure and dimensions of Si membrane structures for use in high-performance lithium ion batteries.