A conventional Ni + YSZ/YSZ anode half-cell (the Research Center Jülich) and the Ni + YSZ/YSZ planar half cell washcoated by a layer of the Ru + Ni-doped perovskite-based nanocomposite (Ru + Ni/LaPrMnCr/YSZ) were compared in terms of their activities and selectivities in the steam reforming of methane. The kinetic measurements were carried out in a laboratory scale plate-type reactor, and results were interpreted using computational models. A power-law kinetic model was verified against the experimental data, and parameters were estimated. Both numerical prediction and experimental testing indicate that the nanocomposite coated Ni + YSZ/YSZ plate shows much better catalytic performance under the middle-temperature operating conditions. CFD simulations show that for the high activity of thermally conductive catalytic plates, superior heat transfer performance is observed in the lab-scale reactor. The lab-scale data were successfully up-scaled for the case of steam reforming of natural gas on a structured catalyst at realistic operation conditions. Up to 700°C, the pilot test data obtained with the structured catalyst comprised of three stacked parallel Ni-Al plates (50 × 50 × 1 mm) coated with perovskite-based nanocomposite correlate quite good with the 1-D plug-flow reactor model predictions assuming the proposed kinetics.