Cost-effective cathodes that actively catalyze the oxygen reduction reaction (ORR) are one of the major challenges for the technological advancement of low-temperature solid oxide fuel cells (LT-SOFCs). In particular, cobalt has been an essential element in electrocatalysts for efficiently catalyzing the ORR; nevertheless, the cost, safety, and stability issues of cobalt in cathode materials remain a severe drawback for SOFC development. Here, we demonstrated that by appropriate nanoengineering, we can overcome the inherent electrocatalytic advantages of cobalt-based cathodes to achieve comparable performance with a cobalt-free electrocatalyst on a bismuth-based fast oxygen ion-conducting scaffold that simultaneously enhances the performance and stability of LT-SOFCs. Consequently, the peak power density of the SOFCs reaches 1.2 W/cm at 600 °C, highest performance of a cobalt-free-based cathode that has been ever reported. In addition, by the surface-protecting effect of covered nanoelectrocatalysts, the evaporation of highly volatile bismuth is greatly suppressed, resulting in an 80% improvement in performance durability, the best among all reported bismuth-based fuel cells.