This study aims to compare two widely used methods of original data collection in nonprofit research: web and mail surveys. We employ an experimental design to assign a web-based survey and a mail survey to nonprofit professionals working in human services organizations in New Jersey. We then compare responses generated from the two survey methods in terms of response rates and data quality. Our study finds that the mail survey achieved a significantly higher response rate than the web survey, and data obtained from the mail survey produced higher internal consistency than that obtained from the web survey. There was no difference between methods, however, in respondent characteristics, the completeness of the survey, and the percentage of missing items. Taken together, the findings suggest that a mail survey, although more costly, may have response-rate and data-quality advantages over a web survey as a methodology for gathering data from nonprofit organizations.