Low-mass dense cores represent the state of molecular gas associated with the earliest phases of low-mass star formation. Such cores are called protostellar or starless, depending on whether they do or do not contain compact sources of luminosity. In this chapter, the first half of the review of low-mass dense cores, we describe the numerous inferences made about the nature of starless cores as a result of recent observations, since these reveal the initial conditions of star formation. We focus on the identification of isolated starless cores and their internal physical and chemical properties, including morphologies, densities, temperatures, kinematics, and molecular abundances. These objects display a wide range of properties since they are each at different points on evolutionary paths from ambient molecular cloud material to cold, contracting, and centrally concentrated configurations with significant molecular depletions and, in rare cases, enhancements.