Increasing agricultural productivity while ensuring environmental sustainability are two important targets in achieving the sustainable development goals under climatic shocks. In this regard, different climate-smart agricultural (CSA) practices have been recommended and promoted to meet these goals and targets. However, the adoption of these practices remains low and variable. For the most part, low adoption has been attributed to external factors. Behavioural and psychological factors also matter but have received little empirical and policy attention. In this study, we examine the relationship between aspirations, aspiration gaps, and the adoption of CSA practices such as crop rotation, intercropping, fallowing, and organic soil amendments. Employing parametric and non-parametric estimation techniques on a pooled farm household survey from Cameroon and Kenya, we show that aspirations are associated with the use of crop rotation and organic soil amendments. We also investigate the theorized non-monotonic inverse U-shaped relationship between aspiration gaps and investments. We find evidence of this relationship for the adoption of these CSA practices, suggesting an aspiration failure for smallholder farmers. These results imply that aspirations that are ahead but not too far ahead of the current state serve as the best incentives for stimulating the adoption of CSA practices. Employing the multivariate probit model, we further highlight interdependencies in the use of these CSA practices. Specifically, we underscore significant complementarities, suggesting the bundled use of these practices. Overall, the analysis demonstrates that aspirations matter for farmer decision-making with many implications for agricultural, food, and environmental policies.