Limited information is available regarding chemical water quality at the tap in Guatemala City, preventing individuals, water utilities, and public health authorities from making data-driven decisions related to water quality. To address this need, 113 participants among households served by a range of water providers across the Guatemala City metropolitan area were recruited as participatory scientists to collect first-draw and flushed tap water samples at their residence. Samples were transported to the U.S. and analyzed for 20 metals and 25 per- and polyfluoroalkyl substances (PFAS). At least one metal exceeded the Guatemalan Maximum Permissible Limit (MPL) for drinking water in 63% of households (n = 71). Arsenic and lead exceeded the MPL in 33.6% (n = 38) and 8.9% (n = 10) of samples, respectively. Arsenic was strongly associated with groundwater while lead occurrence was not associated with location, water source, or provider. One or more PFAS were detected in 19% of samples (n = 21, range 2.1–64.2 ppt). PFAS were significantly associated with the use of plastic water storage tanks but not with location, water source, or provider. Overall, the high prevalence of arsenic above the MPL in Guatemala City tap water represents a potential health risk that current water treatment processes are not optimized to remove. Furthermore, potential contaminants from premise plumbing and storage, including lead and PFAS, represent additional risks requiring further investigation and public engagement.