Ernst Friedrich Ferdinand Zermelo (1871–1953) transformed the set theory of Cantor and Dedekind in the first decade of the 20th century by incorporating the Axiom of Choice and providing a simple and workable axiomatization setting out generative set-existence principles. Zermelo thereby tempered the ontological thrust of early set theory, initiated the delineation of what is to be regarded as set-theoretic, drawing out the combinatorial aspects from the logical, and established the basic conceptual framework for the development of modern set theory. Two decades later Zermelo promoted a distinctive cumulative hierarchy view of models of set theory and championed the use of infinitary logic, anticipating broad modern developments. In this paper Zermelo's published mathematical work in set theory is described and analyzed in its historical context, with the hindsight afforded by the awareness of what has endured in the subsequent development of set theory. Elaborating formulations and results are provided, and special emphasis is placed on the to and fro surrounding the Schröder-Bernstein Theorem and the correspondence and comparative approaches of Zermelo and Gödel. Much can be and has been written about philosophical and biographical issues and about the reception of the Axiom of Choice, and we will refer and defer to others, staying the course through the decidedly mathematical themes and details.