Processing of Gd2Zr2O7 by atmospheric plasma spraying (APS) is challenging due to the difference in vapor pressure between gadolinia and zirconia. Gadolinia is volatilized to a greater extent than zirconia and the coating composition unfavorably deviates from the initial stoichiometry. Aiming at stoichiometric coatings, APS experiments were performed with a TriplexPro plasma torch at different current levels. Particle diagnostics proved to be an effective tool for the detection of potential degrees of evaporation via particle temperature measurements at these varied current levels. Optimized spray parameters for Gd2Zr2O7 in terms of porosity and stoichiometry were used to produce double-layer TBCs with an underlying yttria-stabilized zirconia (7YSZ) layer. For comparison, double layers were also deposited with relatively high torch currents during Gd2Zr2O7 deposition, which led to a considerable amount of evaporation and relatively low porosities. These coatings were tested in thermal cycling rigs at 1400 degrees C surface temperature. Double layers manufactured with optimized Gd2Zr2O7 spray parameters revealed very good thermal cycling performance in comparison to standard 7YSZ coatings, whereas the others showed early failures. Furthermore, different failure modes were observed; coatings with long lifetime failed due to TGO growth, while the coatings displaying early failures spalled through crack propagation in the upper part of the 7YSZ layer.