Energy use due to automobile tires accounts for more than 6% of the world's total energy consumption and ~5% of all carbon dioxide emissions. We designed and fabricated a next-generation, energy-saving advanced elastomer (AE) based on a macromolecular assembly strategy. This AE delicately balances rolling resistance, wear resistance and wet-skid resistance, addressing the so-called “magic triangle” that has plagued the tire industry for more than century. This AE crosslinks anionically synthesized hydroxyl-terminated solution-polymerized styrene-butadiene copolymers with highly symmetric isocyanates and polyols to generate a uniform network by macromolecular self-assembly. Remarkably, compared with those of widely commercialized elastomer nanocomposites tailored for “green tires”, the wear resistance, rolling resistance and wet-skid resistance of this AE are improved by 94.6%, 69.8% and 13.8%, respectively. This AE affords a new opportunity for the large-scale application of next-generation high-performance automobile tires that will, in part, resolve a serious global energy and environmental crisis.