Altmetric indicators are increasingly present in the research landscape. Among this ecosystem of heterogeneous indicators, social reference managers have been proposed as indicators of broader use of scholarly work. However, little work has been done to understand the data underlying this indicator. The present work uses a large-scale survey to study the users of two prominent social reference managers—Mendeley and Zotero. The survey examines demographic characteristics, usage of the platforms, as well as attitudes towards key issues in scholarly communication, such as open access, peer review, privacy, and the reward system of science. Results show strong differences between platforms: Mendeley users are younger and more gender-balanced; Zotero users are more engaged in social media and more likely to come from the social sciences and humanities. Zotero users are more likely to use the platform’s search functions and to organize their libraries, while Mendeley users are more likely to take advantage of some of the discovery and networking features—such as browsing papers and groups and connecting with other users. We discuss the implications of using metrics derived from these platforms as impact indicators.