Laser-cooled and trapped atomic ions form an ideal standard for the simulation of interacting quantum spin models. Effective spins are represented by appropriate internal energy levels within each ion, and the spins can be measured with near-perfect efficiency using state-dependent fluorescence techniques. By applying optical fields that exert optical dipole forces on the ions, their Coulomb interaction can be modulated to produce long-range and tunable spin-spin interactions that can be reconfigured by shaping the spectrum and pattern of the laser fields in a prototypical example of a quantum simulator. Here the theoretical mapping of atomic ions to interacting spin systems, the preparation of complex equilibrium states, and the study of dynamical processes in these many-body interacting quantum systems are reviewed, and the use of this platform for optimization and other tasks is discussed. The use of such quantum simulators for studying spin models may inform our understanding of exotic quantum materials and shed light on the behavior of interacting quantum systems that cannot be modeled with conventional computers.