Systems Thinking (ST) can be defined as a mental construct that recognises patterns and connections in a particular complex system to make the “best decision” possible. In the field of sustainable agriculture and climate change, higher degrees of ST are assumed to be associated with more successful adaptation strategies under changing conditions, and “better” environmental decision making in a number of environmental and cultural settings. Future climate change scenarios highlight the negative effects on agricultural productivity worldwide, particularly in low-income countries (LICs) situated in the Global South. Alongside this, current measures of ST are limited by their reliance on recall, and are prone to possible measurement errors. Using Climate-Smart Agriculture (CSA), as an example case study, in this article we explore: (i) ST from a social science perspective; (ii) cognitive neuroscience tools that could be used to explore ST abilities in the context of LICs; (iii) an exploration of the possible correlates of systems thinking: observational learning, prospective thinking/memory and the theory of planned behaviour and (iv) a proposed theory of change highlighting the integration of social science frameworks and a cognitive neuroscience perspective. We find, recent advancements in the field of cognitive neuroscience such as Near-Infrared Spectroscopy (NIRS) provide exciting potential to explore previously hidden forms of cognition, especially in a low-income country/field setting; improving our understanding of environmental decision-making and the ability to more accurately test more complex hypotheses where access to laboratory studies is severely limited. We highlight that ST may correlate with other key aspects involved in environmental decision-making and posit motivating farmersviaspecific brain networks would: (a) enhance understanding of CSA practices (e.g.,viathe frontoparietal network extending from the dorsolateral prefrontal cortex (DLPFC) to the parietal cortex (PC) a control hub involved in ST and observational learning) such as tailoring training towards developing improved ST abilities among farmers and involving observational learning more explicitly and (b) motivate farmers to use such practices [e.g.,viathe network between the DLPFC and nucleus accumbens (NAc)] which mediates reward processing and motivation by focussing on a reward/emotion to engage farmers. Finally, our proposed interdisciplinary theory of change can be used as a starting point to encourage discussion and guide future research in this space.