Neuroimaging has been a dominant force in guiding research into psychiatric and neurodevelopmental disorders for decades, yet researchers have been unable to formulate sensitive or specific imaging tests for these conditions. The search for neuroimaging biomarkers has been constrained by limited reproducibility of imaging techniques, limited tools for evaluating neurochemistry, heterogeneity of patient populations not defined by brain-based phenotypes, limited exploration of temporal components of brain function, and relatively few studies evaluating developmental and longitudinal trajectories of brain function. Opportunities for development of clinically impactful imaging metrics include longer duration functional imaging data sets, new engineering approaches to mitigate suboptimal spatiotemporal resolution, improvements in image post-processing and analysis strategies, big data approaches combined with data sharing of multisite imaging samples, and new techniques that allow dynamical exploration of brain function across multiple timescales. Despite narrow clinical impact of neuroimaging methods, there is reason for optimism that imaging will contribute to diagnosis, prognosis, and treatment monitoring for psychiatric and neurodevelopmental disorders in the near future.