Self-report instruments of psychological symptoms are increasingly used in counseling centers but rely on rigorous evaluation of their clinical validity. Three studies reported here (total N = 26,886) investigated the validity of the Counseling Center Assessment of Psychological Symptoms-62 (CCAPS-62; Locke et al., 2011) as an assessment and screening instrument. In Study 1, initial evidence regarding the concurrent validity of the CCAPS-62 was replicated and extended in a naturalistic clinical sample of clients from 16 counseling centers. Using this sample, convergent validity of the subscales was examined in counseling center clients, the range of sensitivity of the subscales was investigated using item-response theory, and the presence of 2nd-order factors was preliminarily examined. In Study 2, 7 of the 8 CCAPS-62 subscales statistically significantly differentiated between students in counseling and those who were not, using data collected from a large national survey, although most differences were small and the groups' distributions overlapped considerably. Cut scores based on the differences between these clinical and nonclinical populations showed limited utility due to overall similarities between these broadly defined groups. In Study 3, therapist-rated diagnoses collected from 5 university counseling centers were used to further examine the validity of subscale scores. In addition, cut points for diagnostic screening using receiver operating characteristic curves were evaluated. Overall, these studies support the use of the CCAPS-62 as an initial measure of psychological symptoms in college counseling settings, provide additional information about its psychometric performance, develop cut scores, and illustrate the potential for collaboration between practitioners and researchers on a large scale.