High-yield, chromatography-free syntheses of a ferrocene-templated molecular cage and its Pd-bearing derivative are presented. The formation of a symmetric cage-type structure was confirmed by single-crystal X-ray diffraction analysis. The Pd-bearing cage was used as an innovative catalyst for the efficient synthesis of 1,1′-biphenyls under mild conditions. The presented catalyst is reusable and 1,1′-biphenyls can be obtained efficiently in a gram scale process.