We used the Moving to Opportunity (MTO) housing experiment to inform how Housing Choice Vouchers and housing mobility policies can assist families living in high-poverty areas to make opportunity moves to higher quality neighborhoods, across a wide range of neighborhood attributes. We compared the neighborhood attainment of the three randomly assigned MTO treatment groups (low-poverty voucher, Section 8 voucher, control group) at 1997 and 2002 locations (4-7years after baseline), using survey reports, and by linking residential histories to numerous different administrative and population-based data sets. Compared with controls, families in low-poverty and Section 8 groups experienced substantial improvements in neighborhood conditions across diverse measures, including economic conditions, social systems (e.g., collective efficacy), physical features of the environment (e.g., tree cover) and health outcomes. The low-poverty voucher group, moreover, achieved better neighborhood attainment compared with Section 8. Treatment effects were largest for New York, New York, and Los Angeles, California. We discuss the implications of our findings for expanding affordable housing policy.