Unsafe drinking water is a leading cause of morbidity and mortality, especially among young children in low-income settings. We conducted a national survey in Rwanda to determine the level of faecal contamination of household drinking water and risk factors associated therewith. Drinking water samples were collected from a nationally representative sample of 870 households and assessed for thermotolerant coliforms (TTC), a World Health Organization (WHO)-approved indicator of faecal contamination. Potential household and community-level determinants of household drinking water quality derived from household surveys, the 2012 Rwanda Population and Housing Census, and a precipitation dataset were assessed using multivariate logistic regression. Widespread faecal contamination was present, and only 24.9% (95% CI 20.9–29.4%, n = 217) of household samples met WHO Guidelines of having no detectable TTC contamination, while 42.5% (95% CI 38.0–47.1%, n = 361) of samples had > 100 TTC/100 mL and considered high risk. Sub-national differences were observed, with poorer water quality in rural areas and Eastern province. In multivariate analyses, there was evidence for an association between detectable contamination and increased open waste disposal in a sector, lower elevation, and water sources other than piped to household or rainwater/bottled. Risk factors for intermediate/high risk contamination (> 10 TTC/100 mL) included low population density, increased open waste disposal, lower elevation, water sources other than piped to household or rainwater/bottled, and occurrence of an extreme rain event the previous day. Modelling suggests non-household-based risk factors are determinants of water quality in this setting, and these results suggest a substantial proportion of Rwanda's population are exposed to faecal contamination through drinking water.