This investigation, based on empirical research, examined the role of complexity and order in the aesthetic experience of architectural forms. The basic assumption of this study was that perception in architectural form is a process of interpreting a pattern in a reductive way. Thus, perceptual arousal is not determined by the absolute complexity of a configuration. Rather, the actual perceived complexity is a function of the organization of the system (order). In addition, complexity and order were defined and categorized into four variables according to their significant characteristics; simple order, complex order, random complexity, and lawful complexity. The series of experiments confirmed that there is a point on the psychological complexity dimension which is optimal. By demonstrating that consensual and individual aesthetic preference can be measured to have a unimodal function of relationship with complexity, the results of the experiments indicated that complexity and orderliness are effective design factors for enhancing aesthetics of a building facade. This investigation offered a conceptual framework that relates the physical (architectural form) and psychological factors (complexity and order) operating in the aesthetic experience of building facades.