Rising adult mortality is an essential feature of the mortality transition. Vulnerability to disease and infection decreases with age, and adult mortality is more likely to be from unnatural causes such as suicide, homicide and road traffic accidents. This study aimed to assess the patterns of unnatural deaths in India as a whole and for various population subgroups. Data were obtained from the fourth wave of the National Family Health Survey (NFHS-4) conducted in 2015–16 in 29 states and 7 union territories of India. The survey collected information on deaths in households occurring in the 3 years before the survey. Rate of unnatural mortality and years of life lost were calculated separately for males and females as well as for urban and rural populations. Unnatural mortality in India was found to make up 10.3% of total deaths, and was greater among the population aged 10 to 45 years. The unnatural mortality rate in India was 0.67 per 1000 population: 0.84 per 1000 among the male population and 0.49 per 1000 among the female population. A strict positive association was found between the unnatural mortality rate and a state’s development level. In addition, a substantial loss of person-years of life due to unnatural mortality was observed. The results serve as a reminder of the need to adopt measures to reduce this avoidable loss of life in India. Prevention strategies should be targeted at the most vulnerable populations to limit young-age fatality, with its resulting loss of productive years of life.