The purpose of this study was to validate a novel reading comprehension assessment for college students named MOCCA-College. A random sample of college students (N = 63, average age of 22.5) were recruited from various education programs (e.g., first-year courses, TRIO, SONA) and completed MOCCA-College Online and were later recruited to complete face-to-face think-aloud and recall tasks, as well as standardized assessments such as the Nelson-Denny Reading Test (NDRT) and the Test of Word Reading Efficiency (TOWRE-2). Based on the think-aloud findings, correct answers on MOCCA-College were associated with meaningful connections to background knowledge. Incorrect answers were associated with irrelevant connections to background knowledge that are not helpful for comprehension. Moreover, efficiency on MOCCA-College (seconds per correct answer) demonstrated criterion validity based on the NDRT and TOWRE-2. Future research and analyses may examine assessment development, particularly for identifying nuanced individual differences in college readers' comprehension.