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The BINOL‐derived chiral phosphoric acid (R)‐TRIP is utilized as an organocatalyst in the asymmetric isoprenylboration reaction of aldehydes, wherein hydrogen‐bond interactions play a key role in the control of enantioselectivity. A wide arrays of enantioenriched dienyl homoallyl alcohols, including two natural products (−)‐Ipsdienol and (−)‐Ipsenol, have been successfully constituted. The synthetic...