The museum lives in two connected buildings near the corner of Karyatidon and Kallisperi streets. The larger one, at 12 Kallisperi Street, belongs to the Athenian modernist movement of the 1930s, and from 1968 until the museum opened it held the workshops of Ilias Lalaounis Greek Gold, the first modern jewelry workshops in Greece. The benches where artisans once bent over flames and gold wire now hold display cases. The smaller building facing Karyatidon Street, an Art Deco house from the 1920s, was Lalaounis's own home before it became the museum's offices and research library. The whole complex was renovated in 2003 and 2004, working from plans by the French architect Bernard Zehrfuss.

Lalaounis, born in Athens in 1920, studied economics and law before committing his life to the family trade. His ambition was unusual: not to imitate antiquity with cheap reproductions, but to revive its genuine methods. After analyzing collections across Greece's museums, he and his team mastered hammered gold, granulation, repoussé, and filigree, then paired those ancient skills with modern tools. In 1957 he unveiled his first Archaeological Collection, drawing on Classical, Hellenistic, and Minoan-Mycenaean art. In 1990 the Académie des Beaux-Arts in Paris inducted him as a member, the first and only jeweler ever to receive the honor. He died in 2013, at ninety-three.

The permanent exhibition gathers more than four thousand jewelry pieces and micro-sculptures from fifty collections, all designed by Lalaounis between 1940 and 2002. Some draw on prehistoric art, others on Ancient Greece or the architecture of Byzantium. Fifteen world cultures appear among the designs, alongside collections inspired by nature and even by technology. There are special commissions too, an Olympic torch, ceremonial swords, objects made for a single occasion. Walking the two levels of the exhibition is less a tour of a jewelry shop than a tour of how one obsessive craftsman saw human history, retold entirely in gold.

Lalaounis insisted the museum's first mission be education, not display. It runs programs for schoolchildren from preschool through high school, for adults, and for special-interest and special-needs groups, along with lectures, seminars, and hands-on workshops in jewelry and the decorative arts. University students can apply for internships. The research library holds more than five thousand volumes, some of them rare, covering jewelry, art history, folk art, design, photography, and architecture, and it opens to the public by appointment. Fittingly for a place built around craft for everyone, it was also the first museum in Greece designed to be fully accessible to visitors with disabilities.