High specific surface area carbon aerogel is a kind of adsorption material with excellent comprehensive performance, while its large-scale application is faced with the bottleneck problems including high material cost and complex manufacturing process. Herein, the controllable stripping of the surface micro-scale macropore structure is realized by the control of the activation degree for polyacrylonitrile fiber, the activated fibers with micro-scale macropore structure is completely etched and stripped into three-dimensional frame structured carbon aerogel particles. The prepared carbon aerogel particles have ultra-high surface area (2732.18 m2·g−1) and pore volume (1.13 cm3·g−1) arising almost entirely from micropores (near 90 %), along with abundant surface heterogeneous elements composed by N (10.97 at%) and O (29.67 at%). Attributed to the synergistic effect of physisorption by micropore structure and chemisorption by O/N-containing surface groups, the carbon aerogel particles exhibit excellent hydrogen storage density of 3.17 wt% under ambient pressure. The facile construction strategy for carbon aerogel is proposed from ameliorative activation technology that has been industrialized, which avoids the time-consuming drying process and strict drying conditions in traditional preparation process.