Certain classes of quantum many-body systems, including those supporting phenomena like high-$T_c$ superconductivity and spin liquids, are believed to be fundamentally intractable to classical modeling. Quantum simulations, in which synthetic materials are engineered by inducing well-controlled quantum systems like ultracold atoms to obey many-body Hamiltonians of interest, are a promising new approach to study this type of physics. In this work, I present several advances toward this ultimate goal of large-scale, highly controllable quantum simulations of many-body spin physics. We simulate long-range Ising and XY spin models in the presence of transverse and longitudinal magnetic fields using chains of up to 18 ultracold $^{171}$Yb$^+$ ions held in a linear Paul trap, where two hyperfine levels in each ion encode spin-1/2 states. The tunable spin-spin interactions and effective magnetic fields are engineered using laser fields, and the individual spin states are directly imaged with state-dependent fluorescence. The results in this thesis address several of the ongoing challenges in the development of synthetic quantum matter platforms. One such challenge is establishing more flexible capabilities in the sorts of Hamiltonians we can model. By observing suppression of the ground state spin ordering, we have demonstrated our ability to continuously tune the interaction range in a power-law interaction pattern, and hence the amount of frustration present in the spin system. We have additionally begun developing tools to study particles of higher spin, which could eventually be used to create and study topological phases of matter. Another challenge is the necessity of identifying problems that the next generation of experiments, with flexible (but not arbitrary) controls and classically intractable (but not infinitely large) system sizes, can feasibly shed new light on. We have made measurements of how the range of interaction affects dynamics of spin correlations propagating through the chain, and the excellent agreement between our observations and numerical simulations indicate that at larger sizes, our experiment can meaningfully contribute to the open question of the fundamental speed limit on the transfer of information through such a spin chain. Finally, for classically intractable system sizes, it will be crucial to have multiple techniques at our disposal for validating our understanding of the exact microscopic model being implemented. We have developed and demonstrated an MRI-like spectroscopic technique for probing the energies of the many-body Hamiltonian, which serves as a new method for validating quantum simulations of the transverse Ising model. Our experiments can potentially be scaled up in the near future to study fully connected lattice spin models with several tens of spins, where classical computation begins to fail, and the results described in this thesis contribute to the effort to build experiments that can break new ground in the study of quantum many-body physics.