Functional connectivity studies have demonstrated that creative thinking builds upon an interplay of multiple neural networks involving the cognitive control system. Theoretically, cognitive control has generally been discussed as the common basis underlying the positive relationship between creative thinking and intelligence. However, the literature still lacks a detailed investigation of the association patterns between cognitive control, the factors of creative thinking as measured by divergent thinking (DT) tasks, i.e., fluency and originality, and intelligence, both fluid and crystallized. In the present study, we explored these relationships at the behavioral and the neural level, based on N = 77 young adults. We focused on brain-signal complexity (BSC), parameterized by multi-scale entropy (MSE), as measured during a verbal DT and a cognitive control task. We demonstrated that MSE is a sensitive neural indicator of originality as well as inhibition. Then, we explore the relationships between MSE and factor scores indicating DT and intelligence. In a series of across-scalp analyses, we show that the overall MSE measured during a DT task, as well as MSE measured in cognitive control states, are associated with fluency and originality at specific scalp locations, but not with fluid and crystallized intelligence. The present explorative study broadens our understanding of the relationship between creative thinking, intelligence, and cognitive control from the perspective of BSC and has the potential to inspire future BSC-related theories of creative thinking.