Excessive sitting time and smoking are pro-inflammatory lifestyle factors that are associated with both cancer and cardiovascular disease (CVD) mortality. However, their joint associations have not been investigated. We examined the associations of television (TV) viewing time with cancer and CVD mortality, according to smoking status, among 7,498 non-smokers (34% ex-smokers) and 1,409 current-smokers in the Australian Diabetes, Obesity and Lifestyle Study. During 117,506 person-years (median 13.6 years) of follow-up, there were 346 cancer and 209 CVD-related deaths. Including an interaction between TV time and smoking status in the model significantly improved the goodness of fit for cancer (p=0.01) but not CVD mortality (p=0.053). In the multivariate-adjusted model, every additional hr/d of TV time was associated with increased risk of cancer-related (HR 1.23; 95% CI 1.08-1.40), but not CVD-related mortality (HR 1.16; 95% CI 0.97-1.38) in current-smokers. Elevated multivariate-adjusted cancer mortality HRs were observed for current-smokers watching 2 to <4 hr/d (HR 1.45; 95% CI 0.78-2.71) and ≥4 hr/d (HR 2.26; 95% CI 1.10-4.64), compared to those watching <2 hr/d. Current-smokers watching 2 to <4 hr/d (HR 1.07; 95% CI 0.45-2.53) and ≥4 hr/d (HR 1.92; 95% CI 0.76-4.84) did not have a significantly higher risk of CVD mortality, compared to <2 hr/d. No associations were observed for non-smokers. These findings show an association of TV, a common sedentary behavior, with cancer mortality in current-smokers. The association with CVD mortality was less clear. Further exploration in larger data sets is warranted. Limiting TV viewing time may be of benefit in reducing cancer mortality risk in current-smokers.