Between 1908 and 1911 Perrin published values for Avogadro’s number—the number of molecules per mole of any substance—on the basis of theory-mediated measurements of the mean kinetic energies of granules in Brownian motion. The umbilical cord connecting these energies to Avogadro’s number was the assumption that they are the same as the mean kinetic energies of the molecules in the surrounding liquid. This, as van Fraassen has argued, seems to presuppose that molecules exist, thereby undercutting Perrin’s claim to be proving their existence. This chapter reviews Perrin’s four theory-mediated measurements, showing, on the one hand, that none of them in fact depended on molecular theory yet, on the other, that, by virtue of being exemplars of theory-mediated measurement at its best, they managed to establish several extraordinary landmark conclusions about Brownian motion in its own right.