A growing body of global, evidence-based, research confirms the health, wellness, and academic benefits of childhood exposure to nature. This work explores the feasibility of designing landscape and architectural interventions within primary schools to enhance children’s daily multi-sensorial natural experiences. In Ho Chi Minh City (HCMC), Vietnam, schools have been negatively impacted by issues related to large-scale urban development and by climatic changes. The environmental qualities (both built and natural) have been diminished, and urban pupils are losing their connections with nature in all temporal and spatial dimensions. There is therefore an urgent need to investigate primary school architecture in HCMC in order to provide children with improved educational environments that can provide opportunities for reconnecting them with nature, and to support pro-environmental behaviours. Responding to this, we have developed a research framework with three primary schools in HCMC, as case studies to investigate how various school settings influence child-nature-connection when comprehensively considering how children discover and interact with nature within study and play environments. The study involves observation of children’s interactional behaviours while they are directly experiencing nature. The method has been adopted to examine spatial, psychological, and behavioural dimensions of exposure to nature within educational settings. Results indicate that children’s natural experiences diverge from spatial and natural characteristics in different settings and contexts. Findings offer insights for decision-makers to (re-)create better-suited spaces, with more natural enrichment, to provide an enhanced, diverse, and equitable access to nature for all pupils in their daily activities at schools.