Originally viewed as a few years of apprenticeship and an opportunity to prepare for an independent research career, postdoctoral training has progressed to a state of limbo for some researchers, with longer training durations; uncertain career prospects; and variability in the training, mentoring, and professional status across the neuroscience ecosystem. These challenges have been further exacerbated by the COVID-19 pandemic, resulting in a high level of uncertainty and stress for many postdoctoral researchers. To highlight these challenges and explore opportunities for modernizing postdoctoral training, the Forum on Neuroscience and Nervous System Disorders of the National Academies of Sciences, Engineering, and Medicine held a virtual workshop on February 16, 2021, titled Re-envisioning Postdoctoral Training in Neuroscience. This was the fourth workshop in a series, originating from the Forum’s Action Collaborative on Neuroscience Training: Developing a Nimble and Versatile Workforce, designed to illuminate critical issues and catalyze a reconsideration of how neuroscience training could be designed to meet current and future workforce needs across multiple sectors. This Proceedings of a Workshop-in Brief summarizes the discussions that occurred at the workshop.