Quantum control in large dimensional Hilbert spaces is essential for realizing the power of quantum information processing. For closed quantum systems the relevant inputoutput maps are unitary transformations, and the fundamental challenge becomes how to implement these with high fidelity in the presence of experimental imperfections and decoherence. For two-level systems (qubits) most aspects of unitary control are well understood, but for systems with Hilbert space dimension d>2 (qudits), many questions remain regarding the optimal design of control Hamiltonians 1 and the feasibility of robust implementation 2,3 . Here we show that arbitrary, randomly chosen unitary transformations can be efficiently designed and implemented in a large dimensional Hilbert space (d=16) associated with the electronic ground state of atomic 133 Cs, 4 achieving fidelities above 0.98 as measured by randomized benchmarking 5 . Generalizing the concepts of inhomogeneous control 6 and dynamical decoupling 7 to d>2 systems, we further demonstrate that these qudit unitary maps can be made robust to both static and dynamic perturbations. Potential applications include improved fault-tolerance in universal quantum computation 8 , nonclassical state preparation for high-precision metrology 9 , implementation of quantum simulations 10 , and the study of fundamental physics related to open quantum systems and quantum chaos 11 .The goal of quantum control is to perform a desired transformation through dynamical evolution driven by a control Hamiltonian H C (t) . For example, one common objective is to evolve the system from a known initial state to a desired final state. If the control task is simple or special symmetries are present, it is sometimes possible to find a high-performing control Hamiltonian through intuition, or to construct one using group theoretic methods 12 . In this letter we explore the use of "optimal control" 1 to design control Hamiltonians for tasks of varying complexity, from state-to-state maps to unitary maps on the entire accessible Hilbert space. The basic procedure is well established: the Hamiltonian H C (t) is parameterized by a set of control variables, and a numerical search is performed to find values that optimize the fidelity with which the control objective is achieved. The application of optimal control to quantum systems originated in NMR 13 and physical chemistry 1 , and has since expanded to include, e. g., ultrafast physics 14 , cold atoms 15,16 , biological molecules 17 , spins in condensed matter 18 , and superconducting circuits 19 .We study the efficacy of numerical design and the performance of the resulting control Hamiltonians using a well developed testbed consisting of the electron and nuclear spins of individual 133 Cs atoms driven by radiofrequency (rf) and microwave (µw) magnetic fields (Fig. 1) 16 . Our experiments show that the optimal control strategy is adaptable to a wide range of control tasks, and that it can generate control Hamiltonians with excellent performance even in the prese...