The human brain comprises a multiscale network with multiple levels of organization. Neurons with dendritic and axonal connections form the microscale fabric of brain circuitry, and macroscale brain regions and white matter connections form the infrastructure for system-level brain communication and information integration. In this review, we discuss the emerging trend of multiscale neuroscience, the multidisciplinary field that brings together data from these different levels of nervous system organization to form a better understanding of between-scale relationships of brain structure, function, and behavior in health and disease. We provide a broad overview of this developing field and discuss recent findings of exemplary multiscale neuroscience studies that illustrate the importance of studying cross-scale interactions among the genetic, molecular, cellular, and macroscale levels of brain circuitry and connectivity and behavior. We particularly consider a central, overarching goal of these multiscale neuroscience studies of human brain connectivity: to obtain insight into how disease-related alterations at one level of organization may underlie alterations observed at other scales of brain network organization in mental disorders. We conclude by discussing the current limitations, challenges, and future directions of the field.