At the Cranbook Academy, he met famous artists such as Charles and Ray Eames, Edmund Bacon and Walter Gropius. As the World War II made metal rare and expensive, his artistic talent was mainly channeled into jewelry making. One of the best examples of this productive process was the wedding ring of Ray Eames. Many other examples of his jewelry designs are in prestigious museums all over Europe now.
In 1943 he married Brigitta Valentiner, and then moved to California to work for Charles and Ray Eames at the Molded Plywood Division, learning the key aspects of furniture design. In 1950, he was invited to move to Pennsylvania to work with Hans and Florence Knoll, accomplished furniture producers. During this period he designed five wire pieces that became known as the Bertoia Collection for Knoll. Among these was the famous Diamond Chair (1952), a fluid, sculptural form made from a welded lattice steel structure. Bertoia explained his designs in his own words: "If you look at these chairs, they are mainly made of air, like sculpture. Space passes right through them."
His love and passion for sculpture was finally realized thanks to the royalties he received from these designs at Knoll, which yielded great commercial demand. Reaching the peak of his creative genius, Bertoia started making “Sound Sculpture” and spent the next 25 years experimenting with sound, light and volume through sculptures, paintings and architectural installations. He created a series of innovative sculptures, finding ways to bend and stretch metal so that when crossed with wind or touch, it would create different sounds. Many of Bertoia's “tonal sculptures” were commissioned for established institutions and as public art displays, which are still in place. His smaller pieces of sound furniture or naturalistic works - abstract sculptures that resemble bushes, flowers, leaves or grass- are sought after by affluent collectors and sold at the most prestigious auction houses.