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Tests such as PISA attract speculation about why some countries do well while others do poorly, but limitations of standard methods have precluded systematic examination of this question. We use Qualitative Comparative Analysis (QCA) to examine configurations of conditions that explain national performance on PISA in 34 developed countries. QCA is an innovative approach that is ideal for cross-national comparisons. QCA draws on the strengths of both quantitative and qualitative methods by respecting the diversity and complexity of cases while also identifying generalizable cross-case patterns. While QCA is becoming widespread in the social sciences, this study is among the first to use it in educational research, and offers important insights into the factors contributing to higher achievement in different countries.