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Dendronized hyperbranched polymers (DHPs) can provide advantages for both hyperbranched polymers and dendrimers, making them a promising structure platform for high‐performance second‐order nonlinear optical (NLO) materials. Herein, a new A3+B2‐type DHP (HP2) is reported through facile and efficient [2+2] cycloaddition polymer postfunctionalization, in which tetracyanobutadienyl‐based moieties are...