Atomic spins provide a nearly ideal testbed for exploring protocols in quantum control and measurement, with applications in quantum information processing. Working in collaboration with the experimental group of Poul Jessen at the University of Arizona, Tucson, we have developed a platform for carrying this out based on laser-cooled gases of cesium atoms, controlled and measured with magneto-optical fields. In this talk I will present our recent progress, including optimal control to implement arbitrary unitary transformations in SU(16) and compressed sensing state/process tomography. We can extend these tools to control and measure large atomic ensembles, where light acts as a quantum databus for entangling atoms with one another. I will show how internal atomic state control can be used to strongly enhance the atom-photon entanglement and reach increasingly nonclassical regimes.