Many cognitive self-regulation (CSR) measures are related to the academic achievement of prekindergarten children and are thus of potential interest for school readiness screening and as outcome variables in intervention research aimed at improving those skills in order to facilitate learning. The objective of this study was to identify learning-related CSR measures especially suitable for such purposes by comparing the performance of promising candidates on criteria designed to assess their educational relevance for pre-K settings. A diverse set of 12 easily administered measures was selected from among those represented in research on attention, effortful control, and executive function, and applied to a large sample of pre-K children. Those measures were then compared on their ability to predict achievement and achievement gain, responsiveness to developmental change, and concurrence with teacher ratings of CSR-related classroom behavior. Four measures performed well on all those criteria: Peg Tapping, Head-Toes-Knees-Shoulders, the Kansas Reflection-Impulsivity Scale for Preschoolers, and Copy Design. Two others, Dimensional Change Card Sort and Backwards Digit Span, performed well on most of the criteria. Cross-validation with a new sample of children confirmed the initial evaluation of these measures and provided estimates of test-retest reliability.