The present work aims to boost tourism development in China, grasp the psychology of tourists at any time, and provide personalized tourist services. The research object is the tourism industry in Macau. In particular, tourists' experiences are comprehensively analyzed in terms of dining, living, traveling, sightseeing, shopping, and entertaining as per their psychological changes using approaches including big data analysis, literature analysis, and field investigation. In this case, a model of tourism experience formation path is summarized, and a smart travel solution is proposed based on psychological experience. In the end, specific and feasible suggestions are put forward for the Macau tourism industry. Results demonstrate that the psychology-based smart travel solution exerts a significant impact on tourists' tourism experience. Specifically, the weight of secular tourism experience is 0.523, the weight of aesthetic tourism experience is 0.356, and the weight of stimulating tourism experience is 0.121. Tourists prefer travel destinations with excellent urban security and scenic authenticity. They give the two indexes comprehensive scores of 75.14 points and 73.12 points, respectively. The proposed smart travel solution can grasp the psychology of tourists and enhance their tourism experiences. It has strong practical and guiding significances, which can promote constructing smart travel services in Macau and enhancing tourism experiences.