The present prospect of single-molecule magnets (SMMs) research is more appealing after the detection of magnetic remanence above liquid-nitrogen temperatures. From the current state-of-the-art of the well matured molecular magnetism perspective, in this Review, we discuss the recent emerging trends on the key synthetic strategies employed to achieve exotic magnetic properties by providing representative seminal reports on high-performance Dy­(III)–SMMs (HP-Dy–SMMs). Special emphasis has been given to monomeric HP-Dy–SMMs realized via crystal field (CF), predominant bond, and organometallic approaches. In addition, recent stimulating reports on endometallofullerenes (EMFs) and radical-bridged systems possessing strong magnetic coupling are encompassed. Likewise, the role of spin-vibration coupling in the magnetic relaxation of Dy­(III) MMs is also highlighted. To this end, we believe more demanding theoretical studies are still anticipated to forecast the promising molecule with magnetization blocking at a practical temperature.

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