Unsafe abortion refers to induced abortions performed without trained medical assistance. While previous studies have investigated predictors of unsafe abortion in India, none have addressed these factors with accounting sample selection bias. This study aims to evaluate the contributors to unsafe abortion in India by using the latest National Family Health Survey data conducted during 2019–2021, incorporating the adjustment of sample selection bias. The study included women aged 15 to 49 who had terminated their most recent pregnancy within five years prior to the survey (total weighted sample (N) = 4,810). Descriptive and bivariate statistics and the Heckman Probit model were employed. The prevalence of unsafe abortion in India was 31%. Key predictors of unsafe abortion included women’s age, the gender composition of their living children, gestation stage, family planning status, and geographical region. Unsafe abortions were typically performed in the early stages of gestation, often involving self-administered medication. The primary reasons cited were unintended pregnancies and health complications. This study underscores the urgent need for targeted interventions that take into account regional, demographic, and social dynamics influencing abortion practices in India.