Given educational risks facing Mexican-origin children of immigrant parents, it is important to understand how aspects of the acculturation process influence Mexican-origin youth's educational success. Drawing from selective assimilation theory, this study examined how cultural orientations across myriad facets of acculturation were associated with the educational attainment of second-generation Mexican immigrant youth. The sample included 755 Mexican-origin youth (50% female) in the "Children of Immigrants Longitudinal Study." Results from structural equation models indicated that youth reporting greater facility in the English language and a stronger value on familism attained higher levels of education in young adulthood than did other youth. Parents' U.S. social ties and youth's value on early paid work were associated with less educational attainment. Innovative findings from this study indicate the importance of considering both Mexican and American cultural orientations across myriad facets of acculturation for understanding second-generation immigrant Mexican youth's educational attainment.