Both computer attitude and eLearning self-efficacy are critical complementary factors in determining confidence levels and behavioral belief systems, and can directly affect students' actions, performances and achievements. This study applied a multidimensional construct in validating computer attitude and eLearning self-efficacy of Psychology undergraduate students in Ghana. A sample of students (n = 122) responded to questions on computer attitude anchored on a 5-point scale with high internal consistency reliability coefficients (a = 0.93) and a 4-point scale eLearning self-efficacy (a = 0.84) at p < 0.001. Data were analyzed using ANOVA and correlational statistics. The results validated moderately positive computer attitude of students and high eLearning self-efficacy, with significant variations in both factors. Results of computer attitude sub-levels showed affective (AFF) > perceived usefulness (USE) > behavioral intention (BEH) > perceived control (CON). A bivariate Spearman Spearman correlation between computer attitude and eLearning self-efficacy showed considerable high positive and significant association (r = 0.36), p < 0.05 to suggest that as students' computer attitude increased, so did their eLearning self-efficacy. Mixed effects of demography on both computer attitude and eLearning self-efficacy are reported. A further qualitative inquiry revealed that a blend of online and face-to-face engagements would serve the students' educational needs in the university better.