We present an uncertainty principle for graph signals in the vertex-time domain, unifying the classical time-frequency and graph uncertainty principles within a single framework. By defining vertex-time and spectral-frequency spreads, we quantify signal localization across these domains. Our framework identifies a class of signals that achieve maximum concentration in both the spatial and temporal domains. These signals serve as fundamental atoms for a new vertex-time dictionary, enhancing signal reconstruction under practical constraints, such as intermittent data commonly encountered in sensor and social networks. Furthermore, we introduce a novel graph topology inference method leveraging the uncertainty principle. Numerical experiments on synthetic and real datasets validate the effectiveness of our approach, demonstrating improved reconstruction accuracy, greater robustness to noise, and enhanced graph learning performance compared to existing methods.