The potential health impact of low-level ambient formaldehyde has been historically overlooked. We conducted a two-stage time series analysis to investigate associations between ambient formaldehyde and daily nonaccidental, circulatory, and respiratory mortality and six subtypes based on 5,325,585 deaths in 275 Chinese counties between 2013 and 2018 and estimated a concentration-response curve to identify overall associations. After controlling for confounders from meteorological factors, air pollutants, time trend, and day of the week effect, with a 1-part per billion (ppb) increase in the daily concentration of formaldehyde on lag0 day, we found that mortality risks in nonaccidental, circulatory, and respiratory diseases increased by 0.36%, 0.36% and 0.41%, respectively. The curve indicated a possible threshold concentration at approximately 5 ppb for significant impact on nonaccidental and circulatory diseases. We suggest that ambient formaldehyde may represent a potential threat to public health and needs further investigation to support timely pollution regulation and health protection.