We investigated temporal trends and geographical variations in lung cancer mortality in China from 2006 to 2012. Lung cancer mortality counts for people aged over 40 years were extracted from the China Mortality Surveillance System for 161 disease surveillance points. Negative binomial regression was used to investigate potential spatiotemporal variation and correlations with age, gender, urbanization, and region. Lung cancer mortality increased in China over the study period from 78.77 to 85.63 (1/100,000), with higher mortality rates evident in men compared to women. Median rate ratios (MRRs) indicated important geographical variation in lung cancer mortality between provinces (MRR = 1.622) and counties/districts (MRR = 1.447). On average, lung cancer mortality increased over time and was positively associated with county-level urbanization (relative risk (RR) = 1.15). Lung cancer mortality seemed to decrease in urban and increase in rural areas. Compared to the northwest, mortality was higher in the north (RR = 1.98), east (RR = 1.87), central (RR = 1.87), and northeast (RR = 2.44). Regional differences and county-level urbanization accounted for 49.4% and 8.7% of provincial and county variation, respectively. Reductions in lung cancer mortality in urban areas may reflect improvements in access to preventive healthcare and treatment services. Rising mortality in rural areas may reflect a clustering of risk factors associated with rapid urbanization.