(1) In an era where sustainable behavior is increasingly crucial, understanding the discrepancy between individuals’ sustainability-oriented values and their actual behaviors, known as the inner–outer gap, is vital. This systematic literature review explores the potential of the Tripartite Structure of Sustainability (TSS) framework to address this gap within the context of sustainable education. By reviewing the literature from the APA, ERIC, and Web of Science databases, searched on 25 October 2020, the factors influencing sustainable actions were systematically examined. Articles had to be relevant to the topic (sustainability, morality in relation to sustainability, or morality in general) and report on empirically validated factors that have an impact on the inner-outer gap. (2) By employing a qualitative content analysis approach, 56 articles over a 15-year period were analyzed, identifying 83 factors that either bridged or reinforced the inner–outer gap. These factors were categorized within the TSS framework, which segments sustainability-oriented actions into individual, social, and self-transcendent domains, alongside their activation points: stable, situational, or automated. (3) The analysis revealed that self-focused factors often reinforce the gap, suggesting they are a hindrance to sustainable behavior. Conversely, self-transcendent factors consistently bridged the gap, promoting sustainability. Social factors showed variable impacts based on the ethical and sustainable context they were placed in, suggesting that the social environment’s orientation significantly influences sustainable behavior. (4) This study concludes that the TSS framework offers a promising approach to advancing education for sustainable development (ESD) and contributes insights into how to promote the required paradigm shift towards holistic and interconnected perspectives.

(1) In an era where sustainable behavior is increasingly crucial, understanding the discrepancy between individuals' sustainability-oriented values and their actual behaviors, known as the inner-outer gap, is vital. This study explores the potential of the Tripartite Structure of Sustainability (TSS) framework to address this gap within the context of sustainable education. By reviewing literature from the databases APA, ERIC, and Web of Science, we systematically examined factors influencing sustainable actions. (2) Employing a qualitative content analysis approach, we analyzed 56 articles over a 15-year period, identifying 83 factors that either bridge or reinforce the inner-outer gap. These factors were categorized within the TSS framework, which segments sustainability-oriented actions into individual, social, and self-transcendent domains, alongside their activation points: stable, situational, or automated. (3) Our analysis revealed that self-focused factors often reinforce the gap, suggesting a hindrance to sustainable behavior. Conversely, self-transcendent factors consistently bridged the gap, promoting sustainability. Social factors showed variable impacts based on the ethical and sustainable context they were placed in, suggesting that the social environment's orientation significantly influences sustainable behavior. (4) The study concludes that the TSS framework offers a promising approach to advancing sustainability in education by facilitating a paradigm shift towards holistic and interconnected perspectives. This shift is critical for fostering sustainable behaviors, thereby contributing to the field of educational psychology and offering practical implications for educators aiming to nurture a sustainable future.