<p>We have designed and theoretically investigated a novel binuclear superalkalis H₂M₃ (M = Li and Na) using hydrogen atoms as an electronegative core at the MP2/aug-cc-pVTZ level. These species form diverse geometrical isomers whose superalkali nature has been confirmed by their ionization energy (IE), being lower than the alkali metal atom (5.4–3.9&#xa0;eV). The IE of the lowest energy isomer of H₂M₃ is found to be 3.27 and 3.39&#xa0;eV for M = Li and Na, respectively. The natural population analysis indicates a significant average charge transfer of −0.91<i>e</i> from an alkali metal atom to an individual H-atom. By performing a QTAIM analysis, we reveal the interactions are ionic in these species. We explore the possible applications of the newly designed superalkalis, including the reduction of CO₂ and the formation of stable supersalts. We have analyzed the binding energy of the newly formed H₂M₃-CO₂ clusters and H₂M₃-BF₄ (M = Li and Na) supersalts to assess their stability. These supersalts exhibit significant NLO responses, with <i>α</i>_<i>0</i> and <i>β₀</i> value of 300.72 a.u.&#xa0;and 15,810&#xa0;a.u., respectively. This research seeks to expand the superalkali family and their applications and encourage further studies on these species.</p> Graphical abstract <p></p>