The high‐temperature zirconia electrolyte fuel cell is materials‐limited in both its performance and its range of potential application. The most significant materials limitations and problems occur with the cathode. Cathode materials must satisfy four general criteria: (i) chemical, (ii) electrochemical, (iii) mechanical, and (iv) economical. In this paper, the interaction between cathode materials and cell performance is considered quantitatively for three general classes of cathodes, viz., metals, oxides with embedded current collectors, and electronically conducting oxides.