Angola is one of the countries at the bottom of the ranking in achieving the Sustainable Development Goals (SDGs). Creating sustainable businesses can accelerate the achievement of the SDGs. The present study analyses the antecedents of sustainability-oriented entrepreneurial intention (SOEI) among Angolan higher education students. It starts from the relationships established by the Theory of Planned Behavior (TPB) that were adapted to the sustainable strand. New possible behavioural antecedents of SOEI were added. The Partial Least Square method was applied to a sample of 308 Angolan higher education students. The results show that the TPB dimensions can be adapted and used as antecedents of SOEI and that the TPB can be extended, comprising new antecedents of SOEI also related to individuals' behaviours such as risk-taking propensity, internal locus of control, creativity and proactivity. These unknown antecedents can be taught, learned and stimulated, with universities, policymakers and organisations playing a pivotal role.