Polycyclic aromatic hydrocarbons (PAHs) are widely recognized as catalysts for interstellar H2 formation. Extensive exploration into the catalytic potential of various PAHs has encompassed both theoretical investigations and experimental studies. In the present study, we focused on studying the reactivity of an imperfect aromatic molecule, indene (C9H8), and its hydrogenated counterpart, indane (C9H10), as potential catalysts for H2 formation within the interstellar medium. The reactions of these molecules with H atoms at 3.1 K were investigated experimentally using the para-H2 matrix isolation technique. Our experimental results demonstrate that both indene and indane are reactive toward H atoms. Indene can participate in H-atom-abstraction and H-atom-addition reactions, whereas indane primarily undergoes H-atom-abstraction reactions. The H-atom-abstraction reaction of indene results in the formation of the 1-indenyl radical (R1) (C9H7) and H2 molecule. Simultaneously, an H-atom-addition reaction forms the 1,2-dihydro-indene-3-yl radical (R2) (C9H9). Experiments also reveal that the H-atom-abstraction reaction of indane also produces the R2 radical. To the best of our knowledge, this study represents the first reporting of the infrared spectra of R1 and R2 radicals. The experimental results, combined with theoretical findings, suggest that indane and indene may play a role in the catalytic formation of interstellar H2. Furthermore, these results imply a quasi-equilibrium between the investigated molecules and the formed radicals via H-atom-addition and H-atom-abstraction reactions.