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A dense Ce0.9Gd0.1O2−d (GDC) interlayer is an essential component of the SOFCs to inhibit interfacial elemental diffusion between zirconia‐based electrolytes (eg YSZ) and cathodes. However, the characteristic high sintering temperature of GDC (>1400°C) makes it challenging to fabricate an effective highly dense interlayer owing to the formation of more resistive (Zr,Ce)O2 interfacial solid solutions with YSZ at those temperatures. To fabricate a useful GDC interlayer, we studied the influence of transition metal (TM) (Co, Cu, Fe, Mn, & Zn) doping on the sintering and electrochemical properties of GDC. Dilatometry data showed dramatic drops in the necking and final sintering temperatures for the TM‐doped GDCs, improving the densification of the GDC in the order of Fe > Co > Mn > Cu > Zn. However, the electrochemical impedance data showed that among various transition metal dopants, Mn doping resulted in the best electrochemical properties. Anode supported SOFCs with Mn‐doped, nano, and commercial‐micron GDC interlayers were compared with regard to their performance and stability levels. Although all of the SOFCs showed stable performance, the SOFC with the Mn‐doped GDC interlayer showed the highest power density of 1.14 W cm−2 at 750°C. Hence, Mn‐doped GDC is suggested for application as an effective diffusion barrier layer in SOFCs. [ABSTRACT FROM AUTHOR]