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Do extant levels of social capital in a community influence how an individual uses the Internet and mobile phones and toward what ends, thus making pro-social or anti-social outcomes more likely to result from their use? Rather than consider the effect of Internet and mobile phone use on social capital as the dependent variable, this analysis reorients the causal arrow that has characterized the majority of research to date on this topic. Not only does this provide valuable insight into contextual factors that moderate ICT use and, thus, its effects; it also yields improved understanding of how the overlapping but also unique affordances provided by Internet and mobile phone use will, in some cases, promote different effects on political attitudes and behaviors. This analysis also makes a methodological contribution to the field by leveraging existing data to construct and test more theoretically-appropriate, meso-level measures of social capital.