This study focused on the development of a teacher self-efficacy measurement addressing the contextualization of information and communication technologies (ICTs) with education for sustainability (EfS) using principal component analysis. Furthermore, this study, with the participation of 1815 teachers, examined the predictive value of some hypothesized predictors of the ICTeEfS self-efficacy construct such as gender, school setting, years of teaching, knowledge of education for sustainability, knowledge of ICTs, and experience in using ICTs to support the integration of education for sustainability in teaching and school curricula using multiple regression analysis. The research results revealed that gender did not explain any statistically significant variance of teachers’ ICTeEfS self-efficacy; contrary to this, teachers possessing a high level of knowledge on issues about sustainability and ICT competence explained most of the extracted variance. However, a gap remains in utilizing these skills pedagogically. This study also discusses the varying levels of self-efficacy among teachers based on their workplace location, finding that urban teachers demonstrate higher self-efficacy compared to their rural counterparts. This could be attributed to the disparities in resources and support systems, thereby affecting their capacity to employ ICT in EfS effectively. It was also found that novice teachers exhibited higher predictive power to ICTeEfS self-efficacy, possibly due to their recent exposure to ICT training. This study assumes that a profound understanding of EfS, coupled with ICT tools, bolsters the creation of contextualized curricula and enriches the teaching and learning experience towards sustainability.