materials, which inevitably raises several significant problems in synthetic energy consumption, metal resource crisis, and environmental footprint. [2,3] Against this backdrop, organic materials have become significantly attractive owing to their unique merits of structural diversity, designability, low production cost, and minimum footprint in nature. [4][5][6][7] In the past decade, organic compounds with redox-active centers, including quinones, [8] carboxylates, [9] imines, [10] alkenes, [11] alkynes, [12] azo-, [13] organosulfur-, [7] and radical-groups, [2] have been intensively studied as potential anode/cathode materials for Li-ion batteries and other alkali cation-based batteries. [2,7] As battery researchers are moving in this new direction, it is of much importance to revisit organic electrode materials with a comprehensive perspective for addressing their practical roadblocks. Even though many promising organic electrode materials have been proposed by molecular design, most of them still suffer from low component utilization [14] and sluggish reaction kinetics. [15] It is intrinsically attributed to too localized active sites of charged atoms in specific functional groups such as CX and CXY (X, Y = O, N, S, P). [16] On one hand, the vast majority of organic electrode materials are based on redox chemistry at functional groups, while other components in Organic electrode materials have shown extraordinary promise for green and sustainable electrochemical energy storage devices, but usually suffer from low specific capacity and poor rate capability, which is largely caused by inactive components and diffusion-controlled Li + intercalation. Herein, high-rate Li + intercalation pseudocapacitance in organic molecular crystals is achieved through introducing weak secondary bonding channels, far exceeding their theoretical capacity based on redox chemistry at functional groups. The authors' combined experimentally electrochemical characterization with first-principles calculations show that the heterocyclic organic molecule 2,2′-bipyridine-4,4′-dicarboxylic acid (BPDCA) crystal permits a four-electron redox reaction at conventional CO and CN groups and a six-electron intercalation pseudocapacitance along conjugated alkene hydrogen bonding channels (H 2 NC 5 H⋯OC(OH)) and heterocyclic aromatic stacking channels (C 5 H 3 N⋯NH 3 C 5 ). The BPDCA electrode delivers an ultrahigh reversible capacity of 1206 mAh g -1 at 0.5 A g -1 and an exceptional rate capability. A 4.8 V high-energy/power-density BPDCA anode-based hybrid Li-ion capacitor is thus realized. This work opens a new avenue for developing organic intercalation pseudocapacitive materials via secondary bonding structure design.