Adult illiteracy is a major problem worldwide especially in developing countries. Adult Basic Education (ABE) programs working in this context are not very effective due to lack of motivation for the people who are not literate. The reason is inadequate learning content and content delivery methods. This situation calls for developing novel learning content and a learner-directed content delivery approach. This paper presents an exploratory study investigating the use of the Environmental Print Material (EPM) as learning content for the non-literate population of Pakistan. The EPM content is presented to the adult non-literate population in two ethnographic studies. The most frequently recognized content is selected and utilized as learning content in a Computer Assisted Learning (CAL) application. An empirical study is conducted upon two groups with 107 participants to compare the EPM-based learning content with Traditional Learning Content (TLC). As many as 54 participants participated in the experimental group (presented with EPM-based learning content), whereas 53 participants took part in the control group (presented with TLC content). The results reveal that the experimental group performed significantly better compared to the control group in recognition, pronunciation, and recall of the presented content. The meta-analysis of the results shows a large effect size of (1.05) with confidence interval in the range (0.798–1.315). The results claim that the EPM has potential to be considered as learning content in the ABE programs.