The catalyzed semihydrogenation of dibromomethane (CH 2 Br 2 ) to methyl bromide (CH 3 Br) is a key step in the bromine-mediated upgradation of methane. This study presents a cutting-edge strategy combining density functional theory (DFT), catalytic tests complemented with the extensive characterization of a wide range of metal catalysts (Fe, Co, Ni, Cu, Ru, Rh, Ag, Ir, and Pt), and statistical tools for a computer-assisted investigation of this reaction. The steady-state catalytic tests identified four classes of materials comprising (i) poorly active (<8%) Fe/SiO 2 , Co/SiO 2 , Cu/SiO 2 , and Ag/SiO 2 ; (ii) Rh/SiO 2 and Ni/SiO 2 , which exhibit intermediate CH 3 Br selectivity (<60%); (iii) Ir/SiO 2 and Pt/SiO 2 , which display great propensity to CH 4 (>50%); and (iv) Ru/SiO 2 , which exhibits the highest selectivity to CH 3 Br (up to 96%). In-depth characterization of representative catalysts in fresh and used forms was done by X-ray diffraction, inductively coupled plasma optical emission spectroscopy, N 2 sorption, temperature-programmed reduction, Raman spectroscopy, electron microscopy, and X-ray photoelectron spectroscopy. The dimensionality reduction performed on the 272 DFT intermediate adsorption energies using principal component analysis identified two descriptors that, when employed together with the experimental data in a random forest regressor, enabled the understanding of activity and selectivity trends by connecting them to the energy intervals of the descriptors. In addition, a representative analytic model was found using the Bayesian inference. These findings illustrate the exciting opportunities presented by integrated experimental/computational screening and set the fundamental basis for the accelerated discovery of superior hydrodebromination catalysts and beyond.