Yttria‐stabilized zirconia (YSZ, 8 mol% Y2O3) scaffolds, with surface areas up to 68 m2/g, were prepared by sintering hybrid inorganic‐organic propylene oxide (PO) gels in an argon atmosphere between 1050°C and 1350°C. During sintering, a hard carbon template forms in situ that preserves the scaffold nanomorphology. The carbon template is completely removed postsinter by heating in air to 700°C. Surface areas of 24, 14, 3.2, and 2.4 m2/g were achieved for argon sintering temperatures of 1050°C, 1150°C, 1250°C, and 1350°C, respectively. By adding glucose to the gel formulation, the amount of carbon template increases from 4 to 59 wt% and the surface area increases from 14 to 68 m2/g. Remarkably, the surface area only decreases to 59 m2/g upon heating to 900°C in air. This in situ carbon templating approach offers a flexible platform to create and preserve highly desirable surface areas and nanomorphologies while sintering at high temperatures. The utility of this approach to improve low‐temperature solid oxide fuel cell electrode performance is discussed.