The catalyzed semihydrogenation of dibromomethane (CH2Br2) to methyl bromide (CH3Br) 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/SiO2, Co/SiO2, Cu/SiO2, and Ag/SiO2; (ii) Rh/SiO2 and Ni/SiO2, which exhibit intermediate CH3Br selectivity (<60%); (iii) Ir/SiO2 and Pt/SiO2, which display great propensity to CH4 (>50%); and (iv) Ru/SiO2, which exhibits the highest selectivity to CH3Br (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, N2 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.