The colonias along the United States-Mexico border are generally self-built neighborhoods of low-income families that lack basic infrastructure. While some government assistance has provided roads and electricity, water and wastewater services are still lacking in many colonias. This research is the first to collect a comprehensive dataset on water, sanitation, health, and living conditions in these unincorporated neighborhoods through collection of water samples and surveys; 114 households in 23 colonias across three geographically diverse Texas counties are studied. Water quality is assessed via traditional microbial indicators, chlorine, and arsenic. This complex dataset requires an advanced statistical tool to disentangle relationships among diverse factors. Structural equation modeling is utilized to identify relationships among surveyed and measured variables. The model reveals that colonias residents with well/hauled water accurately predict their water quality, while those with treated+piped water tend to think that their water is worse than it actually is. Dwelling quality and connection to sanitary sewers influence perceived health risks and household health, respectively. Furthermore, these communities have an overwhelming need and desire for point-of-use water treatment. This model can inform decision making and may be adapted to probe other questions and social dynamics for water and sanitation in unincorporated communities elsewhere.