In this review, we report on the formation of a variety of novel, metallic, glassy materials that might well have applications as functional materials. The metallic glasses, with excellent glass‐forming ability, display many fascinating properties and features such as excellent wave‐absorption ability, exceptionally low glass‐transition temperatures (∼35–60 °C) approaching room temperature, ultralow elastic moduli comparable to that of human bone, high elasticity and high strength, superplasticity and polymer‐like thermoplastic formability near room temperature, an excellent magnetocaloric effect, hard magnetism and tunable magnetic properties, heavy‐fermion behavior, superhydrophobicity and superoleophobicity, and polyamorphism, all of which are of interest not only for basic research but also for technological applications. A strategy based on elastic‐moduli correlations for fabrication of bulk metallic glasses (BMGs) with controllable properties is presented. The work has implications in the search for novel metallic glasses with unique functional properties, for advancing our understanding of the nature and formation of glasses, and for extending the applications of the materials.