AbstractThe catalytic reduction of dinitrogen (N2) with dihydrogen (H2) was investigated by means of DFT calculations [MN12‐L/def2‐TZVP(ECP)] using ruthenium pincer complexes of the general formula [Ru{4,6‐bis(di‐tert‐butylphosphanyl)dibenzo[b,d]furan}(H)(X)] (X = H, Me, iPr, Br, I). One tBu group of one of the two phosphorus atoms was augmented with a CH2BH2 group to introduce a borane moiety that is needed for the cooperative stabilization of intermediates and transition states. By optimizing a representative amount of local minima and transition states, it was possible to identify closed catalytic cycles that show surprisingly low activation barriers. As an example, for X = Me after reoptimization in the solvent phase (toluene), transition states with a maximum height in the energy profile of only 36.2 kcal mol–1 were obtained and with the largest single barrier of 29.2 kcal mol–1! It was also observed that the stabilities of amide complexes, which occur late in the catalytic cycle, are very pronounced. Accordingly, they contribute to the overall energy span (ES) in an unfavourable way. However, despite this fact, the calculated ES in the solvent phase for X = I amounts to only 48.4 kcal mol–1 and indicates clearly that the computationally guided design process of the catalyst is a suitable approach to identify elements of a catalyst structure that enables hydrogen‐transfer processes with comparatively low barriers.