The field of quantum science and technology has generated many ideas for new revolutionary devices that exploit the quantum mechanical properties of small-scale systems. Isolated solid state spins play a large role in quantum technologies. They can be used as basic building blocks for a quantum computer or as ultra-sensitive magnetic-field probes which can detect the extremely weak magnetic field generated by a single proton. A major hurdle for realizing these applications is the loss of quantum coherence resulting from uncontrolled interactions with spins in the environment. In the experiments described in my thesis we studied spins associated with defect centers in diamond and used new strategies for mitigating decoherence involving advanced quantum control techniques and for fundamental studies of decoherence. We show that we can prolong the coherence time of a single spin associated with a Nitrogen-Vacancy (NV) defect center in diamond with dynamical decoupling techniques. Our experiments are accurately reproduced theoretically and from this theory we conclude that, with dynamically decoupling, the spin environment can in principle be made irrelevant for the decoherence of a single spin. This removes a major obstacle for using solid-state spins in quantum science and technology. Furthermore, the dynamics in the spin environment and its influence on the NV spin is thoroughly experimentally studied. By better understanding the mechanisms behind decoherence we may one day find the answer to unresolved fundamental issues in quantum physics such as the quantum measurement problem.