Social media data are increasingly used by researchers to gain insights on individuals’ behaviors and opinions. Platforms like Twitter provide access to individuals’ postings, networks of friends and followers, and the content to which they are exposed. This article presents the methods and results of an exploratory study to supplement survey data with respondents’ Twitter postings, networks of Twitter friends and followers, and information to which they were exposed about e-cigarettes. Twitter use is important to consider in e-cigarette research and other topics influenced by online information sharing and exposure. Further, Twitter metadata provide direct measures of user’s friends and followers as opposed to survey self-reports. We find that Twitter metadata provide similar information to survey questions on Twitter network size without inducing recall error or other measurement issues. Using sentiment coding and machine learning methods, we find Twitter can elucidate on topics difficult to measure via surveys such as online expressed opinions and network composition. We present and discuss models predicting whether respondents’ tweet positively about e-cigarettes using survey and Twitter data, finding the combined data to provide broader measures than either source alone.