for use in SIBs due to its small interlayer spacings and inability to generate stable Na-C intercalation compounds. [3] Fortunately, disordered carbonaceous materials with randomly oriented graphitic layers and tunable microstructures have shown great commercialization prospects for SIBs. [4a,b] The electrochemical properties of disordered carbonaceous materials are highly dependent on their microstructures. Based on the degree of graphitization difficulty at high temperature (usually over 2500 °C), disordered carbonaceous materials can be sorted into soft carbon and hard carbon, of which the former displays long-range and highly ordered graphitic layers, while the latter shows a disordered structure with turbostratic domains. [5] In contrast to the low reversible capacity and negligible plateau of soft carbon, hard carbon materials generally exhibit high reversible capacities as well as long and flat plateaus below 0.1 V owing to their large interlayer spacings and disordered pore-rich textures, making them promising for high energy-density SIBs. Hard carbon materials are generally derived from pyrolysis of thermosetting resins, [6a-c] organic macromolecules, [7a-c] biomass, [8a-c] etc., at high temperatures (usually above 1300 °C). The high costs and low yields of these carbon precursors, as well as the complicated and costly production processes, significantly impede practical application. In addition, hard carbon derived from direct pyrolysis of these precursors generally delivers unsatisfactory rate capability, low initial Coulombic efficiency, and poor cycling stability because of the unsuitable sodium ion storage microstructure. [9a,b] Therefore, low-cost and high-yield carbon precursors for hard carbon exhibiting excellent electrochemical performance are highly anticipated.Pitch is a low-cost and abundant byproduct of the petroleum industry, and it is mainly composed of polycyclic aromatic hydrocarbons, which ensures high carbon yield after pyrolysis. [10a,b] Normally, the direct pyrolysis of pitch undergoes an uncontrollable fusion-state carbonization process because of the presence of excess hydrogen and strong π-π interactions between aromatic molecules, resulting in highly graphitized soft carbon with small interlayer spacing. [11] This microstructure ultimately leads to unsatisfactory sodium-ion storage performance, i.e., low reversible capacity and negligible plateau. It has been found that increasing crosslinking of Direct pyrolysis of low-cost and resource-abundant pitch generally produces highly graphitized soft carbon, showing low reversible capacity and a negligible charge-discharge plateau owing to its unsuitable microstructure for sodium storage. Herein, for the first time, an innovative dual-interfering chemistry strategy is proposed to solve the soft-hard carbon translation challenge. Multifunctional zinc gluconate generates dual-mechanism interference upon decomposition and successfully regulates pitch pyrolysis: 1) the gas decomposition products (carbon oxides) may consume excess ...