— In this article, we investigate a new class of control problems called Ensemble Control, a notion coming from the study of complex spin dynamics in Nuclear Magnetic Resonance (NMR) spectroscopy and imaging (MRI). This subject involves controlling a continuum of parameterized dynamical systems with the same open-loop control signal. From a viewpoint of mathematical control theory, this class of problems is challenging because it requires steering a continuum of dynamical systems between points of interest in an infinite dimensional state space by use of the same control function. The existence of such a control raises fundamental questions of ensemble controllability. We introduce the basics of ensemble control and derive the necessary and sufficient controllability characterizations for ensemble control of finite-dimensional time-varying linear systems with an accompanying analytical optimal control law. We show that ensemble controllability is in connection with singular values...