The influence of environmental attitudes on environmental behaviors has long been discussed. However, few studies have addressed the foundation of such attitudes. In the present study, we explored primitive belief underlying environmental attitudes, i.e., connections with nature, and its relationship with pro-environmental behaviors. Specifically, we used scales, a computerized Implicit Association Test, and a situational simulation experiment to examine both explicit and implicit connections with nature, both deliberate and spontaneous environmental behaviors, and to find correlations between environmental connectedness and environmental behaviors. Results showed that explicit connectedness was positively correlated with deliberate environmental behaviors, while implicit connectedness was positively correlated with spontaneous environmental behaviors. Additionally, explicit and implicit connectedness was independent of each other. In conclusion, the current study confirms the positive role played by connections with nature in promoting environmental behavior, and accordingly suggests means to encourage pro-environmental behavior by enhancing people’s connectedness to nature.