In the context of carbon neutrality, it is increasingly important to reduce carbon and increase sinks, and urban green spaces play an important role in carbon sinks. In this paper, we used virtual reality (VR) and photoplethysmographic (PPG) technology to evaluate subject satisfaction regarding urban green space plant community landscape scenes using physiological eye movement and heart rate variability (HRV) data and psychological data obtained according to positive and negative emotional adjectives (PANA). The results of the study showed the following. (1) The physiological data showed the highest visual interest in single-layer grassland. The compound layer of tree-shrub-grass composite woodland communities resulted in the strongest comfort level. (2) The psychological subjective satisfaction evaluation scores were, in descending order: tree-shrub-grass composite woodland (T-S-G) > single-layer grassland (G) > tree-grass composite woodland (T-G) > single-layer woodland (T). (3) The correlation between interest, comfort, and subjective satisfaction was significant, which verified the feasibility of the model of “interest + comfort + subjective evaluation = comprehensive satisfaction”. The results of the study provide theoretical guidance for landscape design based on human perception preferences in the context of carbon neutrality as well as for the implementation of sustainable landscapes to achieve a win–win situation in which carbon sequestration and oxygen release benefits and aesthetics can coexist. The combined physiological and psychological evaluation model can also be applied to other landscapes.