In this paper, we propose a framework for the use of distributed inertial sensors to detect and isolate disturbance sources that might—without subsequent mitigation—have a negative impact on spacecraft pointing accuracy. Common sources of disturbance that have been observed on prior space missions include unbalanced reaction wheels, vibrating cryocoolers, flexing solar panels, and drive mechanisms, among many other examples. Dynamic interactions between disturbance sources like these can lead to micro-vibrations (oscillatory accelerations or specific forces in different parts of the spacecraft structure) and then in turn to jitter (high-frequency angular motion of a sensor). While measurements of jitter often provide little information about disturbance sources, measurements of the underlying micro-vibrations—if made, in particular, by a distributed set of inertial sensors that are co-located with candidate sources of disturbance—could, in principle, reveal which disturbance sources are active or are not behaving nominally and hence are likely to be causing jitter. We derive our framework through analysis of several case studies from prior space missions and show its feasibility through preliminary experiments with a ground-based hardware model.