Motivated by his interest in thermodynamics and the emerging quantum mechanics, Otto Stern (1888–1969) launched in 1919 his molecular beam method to examine the fundamental assumptions of theory that transpire in atomic, molecular, optical, and nuclear physics. Stern’s experimental endeavors at Frankfurt (1919–1922), Hamburg (1923–1933), and Pittsburgh (1933–1945) provided insights into the quantum world that were independent of spectroscopy and that concerned well-defined isolated systems, hitherto accessible only to Gedanken experiments. In this chapter we look at how Stern’s molecular beam research came about and review six of his seminal experiments along with their context and reception by the physics community: the Stern-Gerlach experiment; the three-stage Stern-Gerlach experiment; experimental evidence for de Broglie’s matter waves; measurements of the magnetic dipole moment of the proton and the deuteron; experimental demonstration of momentum transfer upon absorption or emission of a photon; the experimental verification of the Maxwell-Boltzmann velocity distribution via deflection of a molecular beam by gravity. Regarded as paragons of thoroughness and ingenuity, these experiments entail accurate transversal momentum measurements with resolution better than 0.1 atomic units. Some of these experiments would be taken up by others where Stern left off only decades later (matter-wave scattering or photon momentum transfer). We conclude by highlighting aspects of Stern’s legacy as reflected by the honors that have been bestowed upon him to date.