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• Quality of life, notably self-esteem and autonomy, is negatively affected by stopping volunteering. • A variety of benefits were found that can mediate this association, such as satisfaction with transmitting and learning skills. • Initiating volunteering was linked to lower odds of a decrease in material resources satisfaction. • Having financial problem may hinder volunteering. • Support should be provided to promote accessibility and sustainability of volunteering among older adults. The activity theory posits that productive activities are beneficial to older people's well-being. This study examined how quality of life (QoL), globally and in its different dimensions, may be affected by stopping or initiating volunteering, and which psychosocial mechanisms might be at work in such associations. This study used an explicative sequential mixed method design: analyses of 2011 and 2016 data from participants to the Lausanne cohort 65+ (n = 1,976, age 68–77 years in 2011) were followed by qualitative analyses of focus groups made of volunteers participating in the same cohort. Quantitative and qualitative results were then integrated to search for explanations of the former by the latter. Stopping (versus maintaining) volunteering was independently associated with higher odds of a decrease in global QoL and in the "self-esteem and recognition" and "autonomy" dimensions. Observed associations were mediated by the satisfaction of transmitting skills and knowledge, of witnessing the progress of the people being helped, and of feeling useful. Volunteering gave participants a sense of structure and taught them new skills. Initiating volunteering (versus not participating) was independently associated with lower odds of a decrease in the "material resources" dimension and experiencing financial problems was believed to hinder volunteering. Our findings show a positive impact of volunteering on the self-esteem and autonomy of older adults, suggesting that they should be supported in maintaining their volunteer activities. Further exploration of the relationship between material resources and opportunities to volunteer is needed. [ABSTRACT FROM AUTHOR]