Exposure to cadmium, a heavy metal present in cigarettes, can be assessed in both urine and blood. Few studies have compared the properties of concurrent measurements of urine cadmium (uCd) and blood cadmium (bCd) in relation to the duration and timing of a known exposure. In this study, bCd and uCd were modeled with data from the National Health and Nutrition Examination Survey (1999-2010). Adjusted geometric mean bCd and uCd were estimated from regression results. Each 1% higher geometric mean uCd was associated with 0.50% (95% confidence interval: 0.47%-0.54%; R(2)=0.30) higher bCd. In male never-smokers, bCd was 69% (59%-81%) and uCd was 200% (166%-234%) higher at age ≥70 years versus 20-29 years. Ten pack-years (py) of smoking were associated with 13.7% (10.0%-17.4%) higher bCd and 16.8% (12.6%-21.1%) higher uCd in male smokers. The first year after smoking cessation was associated with 53% (48%-58%) lower bCd and 23% (14%-33%) lower uCd in representative males aged 55 years with 20 py smoking. Smoking in the previous 5 days was associated with 55% (40%-71%) higher bCd and 7% (-3%-18%) higher uCd. Results were similar for women. uCd mainly measures long-term exposure and bCd recent exposure, but with noticeable overlap. Epidemiological studies should base the choice of uCd or bCd on the timing of cadmium exposure relevant to the disease under study.