Due to the multiple benefits on energy, well-being, comfort, and the economy, the utilization of daylight remains an imperative topic of architectural design. With the remarkable ability of drawing and increasing daylight deep into the core of buildings, atriums with a large proportion of glazing have become one of the most preferred design forms. The concomitant and unexpected visual discomfort in modern buildings, however, has drawn increasing concerns. Therefore, this study investigated the relation between glazing proportion and daylight performance, as well as the impact of building height and atrium types on daylight performance in atrium buildings by using an annual dynamic simulation method and metrics. It was found that extending glazing proportion had prominent effectiveness in the enhancement of daylighting; building height had a negative influence; round and square types of buildings performed much better than rectangular ones. Moreover, to inform a practical design, we analyzed the link between increasing daylight and visual comfort from the perspective of balancing them, and then proposed a design guide for atrium roof-glazing sizing.