Abstract In the study, the authors addressed two areas of inquiry: the influence of enlisting three underlying cognitive learning processes in alphabet learning, and order effects for letter name and letter sound instruction. Alphabet instruction was designed to enlist paired-associate learning (PAL) only, PAL plus orthographic learning, or PAL plus articulatory learning. Subjects were 94 preschool children, including 35 dual-language learners, in eight public preschool classrooms with low-income eligibility thresholds. Children were randomly assigned within each classroom to small groups that were randomly assigned to one of the three treatments and to one of two orders in which letter names and letter sounds were taught. Research assistants provided 10 weeks of instruction for 12–15 minutes per day, four days a week. All children in the three treatments made significant growth from pretest to posttest on all measures of alphabet learning. Children in the PAL-only condition had significantly higher gains than the sample average on four of the five alphabet measures. Post hoc tests showed that PAL only significantly outperformed the other two conditions on four of the five measures but only for native English-speaking children. No evidence of differences among treatments was found for dual-language learners. Additionally, there was no main effect for order of letter name or letter sound instruction, although teaching letter sounds before letter names was statistically significantly better in the PAL-only treatment. Findings support explicit alphabet instruction emphasizing the relation between verbal letter labels and letter forms that enlists PAL processes.