The level of electronic correlation has been one of the key questions in understanding the nature of superconductivity. Among the iron-based superconductors, the iron chalcogenide family exhibits the strongest electron correlations. To gauge the correlation strength, we performed a systematic angle-resolved photoemission spectroscopy study on the iron chalcogenide series Fe1+ySexTe1−x (0<x<0.59), a model system with the simplest structure. Our measurement reveals an incoherent-to-coherent crossover in the electronic structure as the selenium ratio increases and the system evolves from a weakly localized to a more itinerant state. Furthermore, we found that the effective mass of bands dominated by the dxy orbital character significantly decreases with increasing selenium ratio, as compared to the dxz/dyz orbital-dominated bands. The orbital-dependent change in the correlation level agrees with theoretical calculations on the band structure renormalization, and may help to understand the onset of superconductivity in Fe1+ySexTe1−x.