Background Population densities of many cities are increasing rapidly, with the potential for impacts on cardiovascular health. This longitudinal study examined the potential impact of population‐density increases in urban areas (urban densification) on cardiovascular risk markers among Australian adults. Methods and Results Data were from the Australian Diabetes, Obesity and Lifestyle Study, in which adult participants’ cardiovascular risk markers were collected in 3 waves (in 1999–2000, 2004–2005, and 2011–2012). We included 2354 participants with a mean age of 51 years at baseline who did not change their residence during the study period. Outcomes were 12‐year changes in waist circumference, weight, systolic and diastolic blood pressure, fasting and 2‐hour postload plasma glucose, high‐density lipoprotein cholesterol, and triglycerides. The exposure was neighborhood population densification, defined as 12‐year change in population density within a 1‐km radius buffer around the participant’s home. Multilevel linear growth models, adjusting for potential confounders, were used to examine the relationships. Each 1% annual increase in population density was related with smaller increases in waist circumference (b=−0.043 cm/y; 95% CI, −0.065 to −0.021 [ P <0.001]), weight (b=−0.019 kg/y; 95% CI, −0.039 to 0.001 [ P =0.07]), and high‐density lipoprotein cholesterol (b=−0.035 mg/ dL per year; 95% CI , −0.067 to −0.002 [ P =0.04]), and greater increases in diastolic blood pressure (b=0.032 mm Hg/y; 95% CI , −0.004 to 0.069 [ P =0.08]). Conclusions Our findings suggest that, at least in the context of Australia, urban densification may be protective against obesity risk but may have adverse effects on blood lipids and blood pressure. Further research is needed to understand the mechanisms through which urban densification influences cardiovascular health.