Rainwater harvesting (RWH) is increasingly utilized today by populations to alleviate water supply issues, particularly in rural, dry environments. Limited research has considered, simultaneously, the numerous factors that contribute to sustainability – for example, social acceptance, water quality, and maintenance needs – of RWH. This research aimed to improve the understanding of factors influencing the sustainability of rainwater harvesting systems for domestic use (DRWHS) through examination of social, water quality, and technical feasibility components. We conducted 50 household surveys and 17 rainwater quality analyses in San Jose Xacxamayo, a rural, semi-arid community in Puebla, Mexico. Results showed that DRWHS are socially accepted primarily because of the presence of existing local skills and knowledge, as well as critical need for water. Results from most of the water quality parameters measured were within World Health Organization (WHO) guidelines for human consumption, with the exception of pH, total coliform, and heterotrophic plate count, which required water treatment prior to consumption. Technical feasibility was the main barrier to the sustainability of DRWHS; highly seasonal rainfall and small roof sizes (averaging 70 m2) resulted in households unable to meet annual water needs. Increasing roof sizes and providing water treatment could ensure DRWHS sustainability in the studied community.