In this work, x(1H‐indol‐2‐yl)benzonitrile; where x = ortho or para were used to synthesize boehmite composites using one‐pot electrochemical method in the presence of NaCl as an electrolyte. The prepared composites were characterized using UV–vis, XRD, SEM, and BET. The measurements showed that the type of substituents (ortho, para) had an effect on the resulting nanostructure of the composites, which appeared in the form of nanosheets and nanoballs. The composites were used as materials to store hydrogen at different temperatures (77, 173, 223, and 273 K) under different pressures (10–90 bar) in order to determine the equilibrium pressure for each nanocomposite. The study demonstrated that the composite boehmite‐ortho‐(1H‐indol‐2‐yl)benzonitrile nano balls has a storage capacity of 3.82 wt% at an equilibrium pressure of 75 bar, while the composite boehmite‐para‐(1H‐indol‐2‐yl)benzonitrile nanosheets have the highest storage capacity of 4.49 wt% and an equilibrium pressure of 45 bar.