Effect of Precursor Structure on Pore Evolution of Pitch‐Derived Porous Carbon Nanoarchitectonics

ABSTRACT Developing high‐performance porous carbons (PCs) requires precise microstructural control, which can be effectively understood within the framework of nanoarchitectonics. Mesophase pitch is considered an ideal precursor for preparing high‐performance PCs. However, the intrinsic impact of precursor micro‐texture, specifically the degree of optical anisotropy remains underexplored. This study systematically investigates the evolution of pore architecture in PCs derived from mesophase pitch with varying mesophase contents. It is demonstrated a strong correlation between the graphitic domain arrangement of mesophase pitch precursor and the activation efficiency of potassium hydroxide (KOH). A moderate mesophase content (30%–60%) is identified as the optimal window, facilitating the formation of a 3D honeycomb‐like robust hierarchically porous network with enhanced specific surface area and balanced pore size distribution. Unlike highly ordered precursors that resist etching or amorphous precursors that suffer structural collapse, the moderate mesophase content precursor enables a synergistic mechanism of intercalation and controlled gasification. These findings provide fundamental insights into the nanoarchitectonics of pitch‐derived PCs and offer a practical criterion for precursor selection in the scalable production of high‐performance PCs.