In addition to the specific surface area, surface topography and characteristics such as the pore size, pore size distribution, and micro/mesopores ratio are factors that determine the performance of porous carbons (PCs) in the fields of energy, catalysis, and adsorption. Based on the mechanism of weight loss of polyaspartic acid at high temperatures, this study provided a new method for adjusting the surface morphology of PCs by changing the cross-linking ratio of the precursor, where cross-linked polyaspartic acid was used as precursor without additional activating agents. N adsorption analysis indicated that the specific surface area of the obtained PCs was as high as 1458 m ·g , of which 1200 m ·g was the contribution of the microporous area and the highest pore volume was 1.13 cm ·g , of which the micropore volume was 0.636 cm ·g . The thermogravimetric analysis results of the precursor, and also the scanning electron microscopy and Brunauer–Emmet–Teller analysis results of the carbonization product confirmed that the prepared PCs presented multilevel pore structure, and the diameters of most pores were 0.78 and 3.97 nm; moreover, the pore size distribution was relatively uniform. This conferred the PCs the ultrahigh hydrogen adsorption capacity of up to 4.52 wt-% at 77 K and 1.13 bar, in addition to their great energy storage and catalytic potential.