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The proximity and orientation of the reacting groups can be different in organic cages from in free solution, thus affecting the selectivity of the reaction. Herein, we reported a synthetic strategy to encapsulate iridium nanoparticles (Ir‐NP@COP1‐T) within organic cages in the homogeneous solution. Ir‐NP@COP1‐T showed good selectivity in the hydrosilylation reaction of alkynes. Our work provides a new perspective to the catalysis field by using soluble microporous cages as support for inorganic nano particles. [ABSTRACT FROM AUTHOR]