Quantum mechanical systems lose coherence through interactions with external environments---a process known as decoherence. Although decoherence is detrimental for most of the tasks in quantum information processing, a substantial degree of decoherence is crucial for boosting the efficiency of quantum processes, for example, in quantum biology. The key to the success in simulating those open quantum systems is therefore the ability of controlling decoherence, instead of eliminating it. Here we focus on the problem of simulating quantum open systems with Nitrogen-Vacancy centers, which has become an increasingly important platform for quantum information processing tasks. Essentially, we developed a new set of steering pulse sequences for controlling various coherence times of Nitrogen-Vacancy centers; our method is based on a hybrid approach that exploits ingredients in both digital and analog quantum simulations to dynamically couple or decouple the system with the physical environment. Our numerical simulations, based on experimentally-feasible parameters, indicate that decoherence of Nitrogen-Vacancy centers can be controlled externally to a very large extend.