We prepared the sequence-controlled block copolymers including poly(1-adamantyl acrylate) (PAdA) and poly(n-butyl acrylate) sequences as the hard and soft segments, respectively, by the organotellurium-mediated living radical polymerization. The thermal, optical, and mechanical properties of the adamantane-containing block copolymers with polar 2-hydroxyethyl acrylate (HEA) and acrylic acid (AA) repeating units were investigated. The microphase-separated structures of the block copolymers were confirmed by the differential scanning calorimetry and atomic force microscopy observations as well as dynamic mechanical measurements. The alpha- and beta-dispersions due to the main-chain and side group molecular motions, respectively, of the hard and soft segments were observed. Their transition temperatures and activation energies increased due to the formation of intermolecular hydrogen bonding by the introduction of the HEA and AA repeating units. The effects of the hydrogen bonding on their tensile elasticity, strength, and strain were also evaluated. (C) 2014 Wiley Periodicals, Inc.