The paper deals with a comparative study of equilibrium and kinetics of phenol adsorption from aqueous solutions by means of commercial activated carbons and semi-cokes, differing in the nature of feedstock, production technology and structural characteristics. The main adsorption parameters are calculated with the usage of Langmuir and Dubinin–Radushkevich equations. The change in the characteristics of the structure and state of the surface of semi-coke P2 as a result of modification is estimated. It was found that phenol adsorption kinetics is described by a pseudo-second-order model. The adsorption rate constants and the coefficient of external diffusion mass transfer are calculated. It is proved that phenol extraction from aqueous solutions presents a mixed-diffusion nature, and the process rate is limited by external mass transfer for 13 min for SKD-515 and 22 min for ABG. To increase the adsorption capacity, the oxidative modification of the semi-coke P2 was carried out. Considering the economic and technological aspects, ABG semi-coke is recognized as a promising sorbent for phenol extraction from aqueous media.