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Problems such as global environmental pollution and climate change have made the public’s desire for nature and closeness to greenery increasingly strong amid rapid urbanization. Improving the ability of experiential environmental interpretation products and services is the basis for national parks to meet the public’s needs, and the evaluation of their effectiveness is a necessary basis for optimizing the quality of environmental interpretation services in response to the current problems of unsynchronized environmental interpretation facilities and service levels. Using Pudacuo National Park as a case study, 365 visitors’ spatio-temporal trajectories with GPS devices and questionnaire data were collected, and the interaction changes of visitors’ external spatiotemporal behaviors and internal emotional experiences were analyzed using cluster analysis, GPS geoprocessing model construction, and emotional mean calculation methods, and the results showed that (1) Pudacuo National Park visitors mainly comprise four types of visitor clusters, which are the sightseeing type, trekking + sightseeing type, cruise type, and hiking + cruise type, as well as four types of spatio-temporal behavior patterns; the differences of visitors’ spatiotemporal behavior patterns are reflected in spatial movement, time allocation, and stopping behavior, and correspond to different emotional experience intensity. (2) Emotional experience value is positively correlated with location stay time, and emotional experience intensity is higher, corresponding to spatio-temporal behavior patterns with longer trajectory distance, longer dwell time, and more stopping behaviors, indicating that environmental services promote longer visitor stopping time and generate high-quality recreation experiences. (3) Finally, we proposed the optimization of environmental interpretation mode according to the spatiotemporal emotional differences of different types of visitor clusters. This study provides a basis for improving the quality of visitor experience and optimizing the quality of environmental interpretation services and provides a useful reference for guiding the construction of high-quality and diverse ecological experiences in national parks.