In this paper, we propose a framework to control brain-wide functional connectivity by selectively acting on the brain's structure and parameters. Functional connectivity, which measures the degree of correlation between neural activities in different brain regions, can be used to distinguish between healthy and certain diseased brain dynamics and, possibly, as a control parameter to restore healthy functions. In this work, we use a collection of interconnected Kuramoto oscillators to model oscillatory neural activity, and show that functional connectivity is essentially regulated by the degree of synchronization between different clusters of oscillators. Then, we propose a minimally invasive method to correct the oscillators' interconnections and frequencies to enforce arbitrary and stable synchronization patterns among the oscillators and, consequently, a desired pattern of functional connectivity. Additionally, we show that our synchronization-based framework is robust to parameter mismatches and numerical inaccuracies, and validate it using a realistic neurovascular model to simulate neural activity and functional connectivity in the human brain.