We present a systematic angle-resolved photoemission spectroscopy study of the substitutiondependence of the electronic structure of Rb0.8Fe2(Se1−zSz)2 (z = 0, 0.5, 1), where superconductivity is continuously suppressed into a metallic phase. Going from the non-superconducting Rb0.8Fe2S2 to superconducting Rb0.8Fe2Se2, we observe little change of the Fermi surface topology, but a reduction of the overall bandwidth by a factor of 2. Hence for these heavily electron-doped iron chalcogenides, we have identified electron correlation as explicitly manifested in the quasiparticle bandwidth to be the important tuning parameter for superconductivity, and that moderate correlation is essential to achieving high TC .PACS numbers: 74.25.Jb, 74.70.Xa, In the current study of iron-based superconductors, one of the challenges is to understand the superconductivity (T C ∼ 30 K) in the heavily electron-doped iron chalcogenides A x Fe 2−y Se 2 (A = alkali metal) despite their lack of the ubiquitous Fermi surface (FS) nesting conditions previously thought to be a key for the ironpnictide superconductivity [1][2][3]. Moreover, an antiferromagnetically ordered insulating phase with a spin S = 2 and moment as large as 3.3 µ B [4] has been discovered to exist in proximity to superconductivity in A x Fe 2−y Se 2 . Subsequently, many theories have been proposed to understand the superconductivity in A x Fe 2−y Se 2 from a strong coupling approach [5][6][7], where superconductivity appears in proximity to a Mott phase. Thereby, it becomes important to determine experimentally the key tuning parameters for superconductivity in this family.However, one of the initial challenges has been to control the stoichiometry of the material composition in the growth process, preventing a systematic way to tune the T C . More recently, it has been shown that substitution of selenium by sulfur can tune and suppress T C continuously [8,9], offering a pathway for systematically studying the emergence of superconductivity in this family.In this Letter, we use angle-resolved photoemission spectroscopy (ARPES) to study the Rb 0.8 Fe 2 (Se 1−z S z ) 2 (z = 0, 0.5, 1) series, where the replacement of selenium by sulfur progressively turns a 32 K superconductor into a non-superconducting metallic phase. In the electronic structure, we observe minimal changes in the FS topology, accompanied by a small change of the total charge carrier concentration.More significantly, from Rb 0.8 Fe 2 S 2 to Rb 0.8 Fe 2 Se 2 , the overall quasiparticle bandwidth is observed to decrease by a factor of 2, signaling a dramatic change in electron correlations. This can be understood by considering the bigger size of the selenium atoms compared to sulfur, which expands the lattice, hence increasing the overall electron correlations. Our results show that for the alkali-metal doped iron chalcogenides, electron correlations as controlled by the bandwidth, rather than charge carrier doping or FS topology, is the important tuning parameter for superconductivity, and moderate correla...