The change from solid oxide fuel cell (SOFC) cathodes with surface path kinetics to mixed conducting cathodes exhibiting a bulk path was one of the most important achievements within the last decade of SOFC research. Also in case of anodes the transition to mixed conducting systems is expected to further increase the performance of SOFCs. A promising material for this application is (La,Sr)(Cr,Mn)O3-d (LSCrM), which provides the opportunity of two possible ways of changing its electronic properties: the Sr-doping on the A-site, the Cr:Mn ratio on the B-site. In this study, LSCrM thin films with both varying Sr content and Cr:Mn ratio were prepared by pulsed laser deposition (PLD). Conductivity measurements on these thin films were carried out in 1 % O2, 100 % O2 as well as H2/H2O (1:1) atmospheres using the Van-der-Pauw-method. The obtained conductivity data are discussed in terms of the material-s defect chemistry. Low Mn contents, for example, decrease the conductivity drastically, most likely due to trapping of charge carriers (electron holes) on the Mn sites. With higher Mn contents, site percolation occurs and much higher conductivities can be obtained. The activation energies for each material-s conductivity are calculated from Arrhenius plots and are discussed referring to the corresponding conductivity. A connection between conductivity and activation energy was found. Higher activation energies correspond to lower conductivities at the probed temperatures. Furthermore, the prepared samples demonstrated stability during the time of the measurement under oxidizing as well as reducing conditions. In the second part of the study selected compositions were also investigated as model-type thin film electrodes on yttria stabilized zirconia (YSZ) electrolytes in H2/H2O atmosphere, using a porous Ni/YSZ counter electrode. Electrochemical behavior was characterized by means of impedance measurements and elementary properties such as electrode polarization resistance are discussed referring to the material-s conductivity. The polarization resistance in humid H2 is less dependent on the total conductivity, however, a rather low resistance was observed for La0.9Sr0.1Cr0.2Mn0.8O3-d electrodes. Therefore, the Mn concentration appears to affect the polarization resistance to a higher extent.