The development of improved rechargeable batteries represents a major technological challenge for this new century, as batteries constitute the limiting components in the shift from petrol (gasoline) powered to electric vehicles, while also enabling the use of more renewable energy on the grid. To minimize the ecological implications associated with their wider use, we must integrate sustainability of battery materials into our research endeavours, choosing chemistries that have a minimum footprint in nature and that are more readily recycled or integrated into a full circular economy. Sustainability and cost concerns require that we greatly increase the battery lifetime and consider second lives for batteries. As part of this, we must monitor the state of health of batteries continuously during operation to minimize their degradation. It is thus important to push the frontiers of operando techniques to monitor increasingly complex processes. In this Review, we will describe key advances in both more sustainable chemistries and operando techniques, along with some of the remaining challenges and possible solutions, as we personally perceive them.