A planar tetranuclear palladium cluster was obtained from the reaction of a cyclotetrasilane with [Pd(CNtBu)2]3. Single‐crystal X‐ray diffraction analysis and DFT calculations revealed that the tetranuclear framework of the cluster was supported effectively by the bridging organosilylene ligand. Although [Pd(CNtBu)2]3 as well as mononuclear palladium bis(silyl) complex, cis‐Pd(SiMePh2)2(CNtBu)2, do not act as the effective catalyst, the planar tetranuclear palladium cluster acts as an efficient catalyst for the hydrogenation of alkenes and alkynes including sterically hindered tri‐ and tetra‐substituted alkenes.

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