This article uses data from the 2006 Social Capital Community Survey to examine the impact of social capital, religious capital, human capital, and attitudes on volunteerism. Five alternative structural models are estimated. Tests reveal unambiguously the inferiority of the Tobit model and point to a double-hurdle model with independent errors as the best alternative. Major findings are that more diversity in friendships and more education increase the likelihood of volunteering, greater intensity of religious belief increases the level of volunteerism, and more informal social networking and formal group involvement along with greater religious participation increase both the likelihood and level of volunteering. Study results suggest strongly that the nonprofit voluntary sector has a vested interest in promoting policies that expand educational opportunities and foster civil engagement, social interaction, and religious participation.